Gasification of plastic and solid fossil fuels

By gasifying the oxidant and raw material composition in the airflow-bed gasification furnace, the problems of incomplete oxidation and synthesis gas composition variation in the waste gasification furnace are solved, and efficient and stable synthesis gas flow production is achieved, which is suitable for chemical synthesis.

CN120118698APending Publication Date: 2025-06-10EASTMAN CHEM CO
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Patent Information

Application Number
CN202510332438.8
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Priority Date
2020-02-03
Filing Date
2020-02-04
Publication Date
2025-06-10

AI Technical Summary

Technical Problem

Existing waste gasifiers operate at low to medium temperatures, resulting in incomplete oxidation reactions, producing a large amount of residues, and the composition of the synthesis gas varies over time, making it difficult to meet the requirements of chemical synthesis.

Method used

Using a gas-flow-bed gasification furnace, the oxidant and feedstock compositions (including solid fossil fuels and up to 25 wt.% of recycled plastic) are gasified at high temperatures to produce a stable and consistent synthesis gas flow.

Benefits of technology

A more complete oxidation reaction is achieved, reducing residue generation, ensuring consistency of the composition of the synthesis gas flow, and is suitable for chemical synthesis.

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Abstract

A small particle size, no greater than 2 mm pre-ground plastic is co-fed into a solid fossil fuel feed entrained flow partial oxidation gasifier. High solids concentrations can be obtained in the feed stream without significantly affecting the stability and pumpability of the feed stream. According to the invention, syngas of consistent quality can be continuously produced, including production of carbon dioxide and carbon monoxide / hydrogen ratios, while stably operating the gasifier, avoiding the fluidized bed or fixed bed waste gasifier from producing high tar, and not affecting the operation of the gasifier. Subsequent syngas produced from the material can be used to produce a wide range of chemicals.
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Description

[0001] This application is a divisional application of a patent application for invention with a priority date of February 4, 2019, a filing date of February 4, 2020, an application number of 202080012483.0, and an invention title of "Gasification of Plastics and Solid Fossil Fuels". Background Art

[0002] There are well-known global problems in waste disposal, especially for a large number of consumer goods such as plastics, textiles, and other polymers, which are considered not to be biodegradable within an acceptable time limit. The public expects to incorporate these types of waste into recycled products by recycling, reusing, or otherwise reducing the amount of waste in circulation or landfills.

[0003] A variety of methods have been proposed for recycling, reusing, or reducing waste such as biomass, solid municipal waste, plastics, and paper, including gasification of these wastes. In these proposals, waste gasifiers have been proposed or used, which are generally air-supplied fluidized bed gasifiers that can easily accept various component sizes and types. Such waste gasifiers typically operate using air as an oxidant at low to medium temperatures in the range of 500 °C to 1000 °C, and at lower operating temperatures, incomplete oxidation reactions occur, resulting in the production of a large amount of residues, which can appear in the gas phase (synthesis gas stream) and the bottom solid phase; for example, tar-like substances. The type and amount of residues will vary according to the feedstock composition. In addition, although waste gasifiers have the advantage of accepting feedstocks with highly variable sizes and compositions, the resulting syngas composition also varies widely over time, such that they cannot be used to manufacture chemicals without installing expensive post-treatment systems to purify and purify the synthesis gas stream present in the gasifier vessel. Even with purification methods, the hydrogen / carbon monoxide / carbon dioxide ratio can still remain highly variable. Due to the cost of installing systems to purify the synthesis gas stream leaving the gasifier vessel for chemical synthesis, or their compositional variability, or their low production volume, or due to a combination of these factors, the synthesis gas streams produced by waste gasifiers are typically used to generate energy, such as steam or electricity.

[0004] The use of recycled plastics as feedstock for gasifiers has been studied. Recycled plastic feedstocks are highly variable. Since plastic feedstocks contain a mixture of plastics with different polymer structures, the composition of the recycled plastic feedstock is variable at any given time. Even feedstocks specified by polymer type can vary in terms of their molecular weight or structure (e.g., LDPE versus HDPE). This problem is complicated by the variability of the feedstock stream composition over time, which depends on seasonality, source location, and the suppliers of such recycled plastic streams, who use a variety of different physical and chemical separation methods. In fixed-bed and fluidized-bed gasifiers, this can lead to unacceptable variability in the syngas composition over time, especially when syngas is required to synthesize chemicals that require very consistent rates and qualities of syngas or syngas components.

[0005] In addition, plastics have a lower fixed carbon content than solid fossil fuel sources such as coal or petroleum coke. As a result, plastics will burn at a faster rate than, for example, coal and produce syngas components. Therefore, relative to coal, the carbon monoxide produced from plastics will have a longer residence time under gasification conditions to convert to carbon dioxide. Although plastics have a higher higher heating value (“HHV”) than or equal to coal, making them an attractive gasifier feedstock, their use can also lead to the production of an undesirable amount of carbon dioxide in the raw syngas stream and a reduction in the amount of carbon monoxide, which would be possible by feeding only fossil fuels. In addition, plastics have a higher hydrogen content than, for example, solid fossil fuels, which can lead to the production of a higher amount of hydrogen in the raw syngas stream and affect the carbon monoxide / hydrogen ratio. These issues are not a concern when syngas is used for power generation or combustion to obtain heat value, but they become a concern when manufacturing chemicals, as the manufacture of chemicals relies on carbon monoxide and / or hydrogen as feedstocks.

[0006] We desire a method for gasifying a plastic stream that will produce a syngas stream suitable for chemical synthesis, in which more complete oxidation of the waste feedstock occurs to reduce the amount of incomplete oxidation residues. We also desire to produce a syngas stream exiting the gasifier vessel that is sufficiently consistent in composition over time and suitable for manufacturing chemicals, and in particular does not require co-blending of syngas streams. It is also desirable to operate in a stable manner and efficiently on a commercial scale.

[0007] While it is desirable to have minimal variation in the syngas composition produced from feedstocks having solid fossil fuels and recycled materials, it is also desirable to have a flexible method in which the recycled materials can be fed intermittently (or semi-continuously) without a large change in the syngas composition between the syngas produced from the feedstock having recycled materials and the syngas produced from the feedstock not having recycled materials.

[0008] We have evaluated the use of a coal-water slurry feed gasifier for producing syngas for chemical production. Coal gasifiers with slurry feeds typically operate at high pressure and utilize a slurry feed (coal and water) that can be more easily pumped and fed into the gasifier. A small amount of water introduced into the gasification process is helpful and necessary (e.g., 5 - 20%), but water in excess of 30% begins to be detrimental to the performance of the gasifier because the water must be heated and gasified using energy and occupies space in the processing equipment. Thus, the slurry should be as concentrated in coal as possible but still have sufficient fluidity to be pumped. The actual range of coal / water slurry concentration is 50% - 75% coal. To enable these concentrations, the coal is finely ground. Introducing a co-feed into the gasifier can be problematic because the co-feed must be mixed with the coal / water slurry feed. For economic reasons, the coal / water slurry is concentrated as much as possible to the edge of pumpability, so the introduction of any co-feed can disrupt the delicate balance and cause the slurry to be unstable (solid settling), too thick, two-phase, or otherwise unsuitable for safely, reliably, and economically feeding into the gasifier. For example, many plastics will float, or phase separate, or agglomerate and disrupt the uniformity of the slurry.

[0009] There is still a need to gasify recycled plastic materials in a stable slurry.

[0010] There is also a need to ensure that such a slurry is pumpable.

[0011] There is still a need to gasify recycled plastics including coal without producing a large amount of tar, or optionally also without producing a large amount of other incomplete oxidation residues, such as would be encountered in a fixed bed or fluidized bed waste gasifier.

[0012] There is also a need to gasify a mixed stream containing recycled plastics to provide a syngas stream with minimal compositional variability over time.

[0013] There is also a need to provide intermittent co-feeding of recycled plastics and solid fossil fuels while including a raw material with and without recycled plastic waste to maintain a minimal syngas compositional variability over a time range.

[0014] There is also a need to produce such a syngas stream that is suitable for manufacturing chemicals and, optionally but desirably, does not require the installation and operation of additional equipment to clean the syngas stream leaving the gasifier vessel other than an acid gas removal process (e.g., removing hydrogen sulfide and carbon dioxide) or a process inside the gasifier vessel (e.g., quenching to remove soot).

[0015] There is also a need to address any combination of the above needs. SUMMARY OF THE INVENTION

[0016] There is now provided a method for producing syngas, comprising:

[0017] a. Load an oxidizer and a feedstock composition into a gasification zone within a gasifier, the feedstock composition comprising a solid fossil fuel and up to 25 wt.%, or up to 20 wt.%, or up to 15 wt.%, or up to 12 wt.%, or up to 10 wt.%, or up to 7 wt.%, or up to 5 wt.%, or less than 5 wt.% recycled plastic, based on the weight of the solids in the feedstock composition;

[0018] b. Gasify the feedstock composition together with the oxidizer in the gasification zone to produce a syngas composition; and

[0019] c. Discharge at least a portion of the syngas composition from the gasifier;

[0020] wherein the gasifier is an entrained flow gasifier.

[0021] There is now provided a method for producing syngas, comprising:

[0022] a. Load an oxidizer and a feedstock composition into a gasification zone within a gasifier, the feedstock composition comprising a solid fossil fuel and 90 wt.% of the recycled plastic having a particle size not greater than 2 mm in the maximum dimension;

[0023] b. Gasify the feedstock composition together with the oxidizer in the gasification zone to produce a syngas composition; and

[0024] c. Discharge at least a portion of the syngas composition from the gasifier;

[0025] wherein the gasifier is an entrained flow gasifier.

[0026] Desirably, the feedstock is a slurry.

[0027] There is further provided a method for producing syngas, comprising:

[0028] a. Load an oxidizer and a feedstock slurry composition into a gasification zone within a gasifier, the feedstock slurry composition comprising recycled plastic, a solid fossil fuel, and water, wherein (i) the amount of recycled plastic is up to 25 wt.%, or up to 20 wt.%, or up to 15 wt.%, or up to 12 wt.%, or up to 10 wt.%, or up to 7 wt.%, or up to 5 wt.%, or less than 5 wt.%, based on the weight of the solids in the feedstock slurry, or (ii) 90 wt.% of the recycled plastic has a particle size not greater than 2 mm in the maximum dimension;

[0029] b. Gasify the feedstock composition together with the oxidizer in the gasification zone to produce a syngas composition; and

[0030] c. At least a portion of the syngas composition is discharged from the gasifier, wherein at least one of the following conditions exists:

[0031] (i) The gasification in the gasification zone is carried out at a temperature of at least 1000 °C, or

[0032] (ii) The pressure in the gasification zone is greater than 2.7 MPa, or

[0033] (iii) The feed composition is a slurry, or

[0034] (iv) No steam is introduced into the gasifier and flows into the gasification zone, or

[0035] (v) The recycled plastic is pre-ground so that at least 90% of the particles have a particle size of less than 2 mm, or

[0036] (vi) The tar yield is less than 4 wt.%, or

[0037] (vii) The gasifier does not contain a membrane wall in the gasification zone, or

[0038] (viii) A combination of two or more of the above conditions.

[0039] The present invention also includes a feedstock slurry composition comprising recycled plastic, solid fossil fuel, and water, wherein the recycled plastic has a particle size of not more than 2 mm, and the solid fossil fuel in the feed composition has a particle size of less than 2 mm, the solid content in the slurry is at least 62 wt.% (or at least 65 wt.%, or at least 68 wt.%, or at least 69 wt.%, or at least 70 wt.%), the amount of recycled plastic present in the feedstock slurry composition is from 0.1 wt.% to at most 25 wt.%, or at most 20 wt.%, or at most 15 wt.%, or at most 12 wt.%, or at most 10 wt.%, or at most 7 wt.%, or at most 5 wt.%, or less than 5 wt.%, based on the weight of all solids, and the amount of water is at least 20 wt.%, based on the weight of the feedstock slurry composition, and wherein:

[0040] a. The slurry is stable, as determined using a Brookfield R / S rheometer operating at a shear rate of 1.83 / s equipped with V80-40 blades or a Brookfield viscometer with an LV-2 spindle rotating at a rate of 0.5 rpm, having an initial viscosity of 100,000 cP or less at 5 minutes, or 10 minutes, or 15 minutes, or 20 minutes, or 25 minutes, or even 30 minutes, measured under ambient conditions; or

[0041] b. The slurry is pumpable, such as after mixing to obtain a uniform distribution of solids throughout the slurry, and has a viscosity of less than 30,000 cP, or not more than 25,000 cP, or not more than 23,000 cP, or not more than 20,000 cP, or not more than 18,000 cP, or not more than 15,000 cP, or not more than 13,000 cP, as determined using a Brookfield R / S rheometer operating at a shear rate of 1.83 / s equipped with V80 - 40 blades or a Brookfield viscometer rotating at a rate of 0.5 rpm equipped with an LV - 2 spindle or a Brookfield R / S rheometer operating at a shear rate of 1.83 / s equipped with V80 - 40 blades or a Brookfield viscometer rotating at a rate of 0.5 rpm equipped with an LV - 2 spindle or a Brookfield R / S rheometer operating at a shear rate of 1.83 / s equipped with V80 - 40 blades or a Brookfield viscometer rotating at a rate of 0.5 rpm equipped with an LV - 2 spindle, measured under ambient conditions, or

[0042] c. Both of the above.

[0043] There is further provided a syngas composition which is discharged from a gasifier and obtained by gasifying a feed stream comprising recycled plastics and solid fossil fuels, wherein (i) the amount of recycled plastics is at most 25 wt.%, or at most 20 wt.%, or at most 15 wt.%, or at most 12 wt.%, or at most 10 wt.%, or at most 7 wt.%, or at most 5 wt.%, or less than 5 wt.%, based on the weight of solids in the feed stream, or (ii) the recycled plastics have a particle size of not more than 2 mm, or (iii) both of the above, and the syngas stream does not contain tar or contains not more than 4 wt.% (or less than 3 wt.%, or not more than 2 wt.%, or not more than 1 wt.%, or not more than 0.5 wt.%, or not more than 0.2 wt.%, or not more than 0.1 wt.%, or not more than 0.08 wt.%, or not more than 0.05 wt.%, or not more than 0.02 wt.%, or not more than 0.01 wt.%, or not more than 0.005 wt.%) of tar, based on the weight of all condensable solids in the syngas composition.

[0044] There is further provided a syngas composition stream which is produced by gasifying a feed (mixed feed) comprising solid fossil fuels and recycled plastics in a gasifier, the feed having a compositional variability of 5% or less measured over the shorter of a 12 - day period or the period during which the mixed feed is fed to the gasifier, the syngas compositional variability being measured and satisfying at least one of the following gaseous compounds (in moles):

[0045] a. The amount of CO, or

[0046] b. The amount of H2, or

[0047] c. The amount of CO2, or

[0048] d. The amount of CH4, or

[0049] e. The amount of H2S, or

[0050] f. The amount of COS, or

[0051] g. The amount of H2 + CO, or their sequential molar ratio (e.g., H2:CO ratio), or

[0052] h. The amount of H2 + CO + CO2, or their sequential molar ratio, or

[0053] i. The amount of H2 + CO + CH4, or their sequential molar ratio, or

[0054] j. The amount of H2 + CO + CO2 + CH4, or their sequential molar ratio, or

[0055] k. The amount of H2S + COS, or their sequential molar ratio, or

[0056] l. H2 + CO + CO 2 +CH 4 +H 2 S + COS.

[0057] There is also provided a syngas combined stream having a switching variability of negative, zero or not greater than 15%, wherein the switching frequency is at least 1x / 2 year and the switching variability is determined by the following equation:

[0058]

[0059] where %SW is the syngas switching variability percentage of one or more measured components in the syngas composition; and

[0060] V m is the syngas composition variability of gaseous compounds using a mixed stream comprising recycled plastics and fossil fuels; and

[0061] V ff is the syngas composition variability of the same gaseous compounds using a stream of only fossil fuels, and wherein the solid concentration is the same in both cases, the fossil fuels are the same in both cases, and the feedstock is gasified under the same conditions, except for possible temperature fluctuations that are different due to the presence of recycled plastics in the feedstock, and the variability is measured and satisfies at least one of the following gaseous compounds (in moles):

[0062] a. The amount of CO, or

[0063] b. H 2 quantity, or

[0064] c. CO2 quantity, or

[0065] d. CH4 quantity, or

[0066] e. H2S quantity, or

[0067] f. COS quantity, or

[0068] g. H2 + CO quantity, or their sequential molar ratio (e.g., H2:CO ratio), or

[0069] h. H2 + CO + CO2 quantity, or their sequential molar ratio, or

[0070] i. H2 + CO + CH4 quantity, or their sequential molar ratio, or

[0071] j. H2 + CO + CO2 + CH4 quantity, or their sequential molar ratio, or

[0072] k. H2S + COS quantity, or their sequential molar ratio, or

[0073] l. H2 + CO + CO 2 + CH 4 + H 2 S + COS. Description of the Drawings

[0074] Figure 1 is a schematic equipment design for combining recycled plastics and solid fossil fuels as raw materials into a gasification process to produce syngas.

[0075] Figure 2 is another example of an equipment design for gasifying raw materials of recycled plastics and solid fossil fuels to produce a washed syngas stream.

[0076] Figure 3 is a cross-sectional view of a gasifier injector.

[0077] Figure 4 is a more detailed view of the nozzle part of the gasifier injector.

[0078] Figure 5 is a detailed view of the location for adding recycled plastics to solid fossil fuels. Detailed Description of the Invention

[0079] Unless otherwise specified, the weight of the indicated raw material stream includes all solids fed to the gasifier, if there are liquids, and unless otherwise specified, does not include the weight of any gas in the raw material stream fed to the injector or gasifier.

[0080] For classifying materials in a feed stream, the fossil fuels used are coal, petroleum coke or any other solid at 25 °C and 1 atmosphere of pressure, which are by-products from refined oil or petroleum. The fossil fuel portion of the feed stream is different from plastics, even though plastics are carbon-containing and derived from raw materials obtained from refined crude oil.

[0081] Typically, in a syngas operation, a feed stream consisting of a finely granulated fossil fuel source (such as coal, petroleum coke), granulated plastics, and optionally water and other chemical additives is injected into the gasification reaction zone or chamber of a syngas generator (gasifier) together with an oxidant gas. A hot gas stream is generated in the reaction zone (desirably lined with refractory), producing slag, ash, soot, and gases including hydrogen, carbon monoxide, carbon dioxide, and depending on the fuel source and reaction conditions, may include other gases such as methane, hydrogen sulfide, and nitrogen. The hot gas stream generated in the reaction zone is cooled using a syngas cooler or a quench water bath at the bottom of the gasifier, which also solidifies the ash and slag and separates the solids from the gas. The quench water bath also acts as a seal to maintain the internal temperature and pressure in the gasifier while transferring the slag, soot, and ash into a lock hopper. The cooled product gas stream (raw syngas stream) removed from the gasifier is further treated with plastics to remove remaining solids and then further treated, optionally after further cooling and adjusting the ratio of carbon monoxide to hydrogen, to remove acid gases (such as hydrogen sulfide).

[0082] The plastics used in the feed stream include any organic synthetic polymer that is solid at 25 °C and 1 atmosphere of pressure. The polymer can be a thermoplastic or thermosetting polymer. The number average molecular weight of the polymer can be at least 300, or at least 500, or at least 1000, or at least 5,000, or at least 10,000, or at least 20,000, or at least 30,000, or at least 50,000, or at least 70,000, or at least 90,000, or at least 100,000, or at least 130,000. The weight average molecular weight of the polymer can be at least 300, or at least 500, or at least 1000, or at least 5,000, or at least 10,000, or at least 20,000, or at least 30,000 or at least 50,000, or at least 70,000, or at least 90,000, or at least 100,000, or at least 130,000, or at least 150,000, or at least 300,000.

[0083] The plastic is recycled plastic, which can be post-consumer plastic and post-industrial plastic, and is usually also referred to as pre-consumer plastic. Post-consumer plastic is plastic that has been used at least once in its intended application at any time, regardless of wear. Post-industrial or pre-consumer plastic includes reprocessed, reground, scrap, trim, off-specification plastic, any plastic that has been synthesized but not used in the final application, or any plastic that has not been used by the end consumer.

[0084] The form of plastic that can be used for grinding and pre-ground plastic is obtained from plastic forms, which are not limited and can include sheets, extruded shapes, molded articles, films, laminates, and foams. Desirably, fabrics are not used as a source for obtaining pre-ground plastic because many fabrics are a mixture of synthetic and natural fibers. Plastics can have different ages and compositions. Incombustible inorganic substances such as metals and minerals that prevent the plastic from burning and emitting can be included in the plastic used for gasification. Examples include tin, cobalt, manganese, antimony, titanium, sodium, calcium, sulfur, zinc, and aluminum, their oxides, and their other compounds. Advantageously, titanium and calcium that may be present in the plastic can be slag modifiers.

[0085] In one embodiment or in combination with any of the embodiments mentioned, the amount of calcium compound present in the ash of the pre-ground plastic used in the feedstock is at least 30 wt.%, or at least 40 wt.%, or at least 50 wt.%, or at least 55 wt.%, or at least 60 wt.%, or at least 63 wt.%, based on the weight of the plastic ash. The upper limit is desirably not greater than 90 wt.%, or not greater than 80 wt.%, or not greater than 75 wt.%, based on the weight of the plastic ash.

[0086] In another embodiment, the amount of sodium compound present in the ash of the pre-ground plastic used in the feedstock is at least 2 wt.%, or at least 3 wt.%, or at least 4 wt.%, or at least 5 wt.%, or at least 6 wt.%, or at least 7 wt.%, based on the weight of the plastic ash. The upper limit is desirably not greater than 20 wt.%, or not greater than 17 wt.%, or not greater than 15 wt.%, based on the weight of the plastic ash.

[0087] In another embodiment, the amount of titanium compound present in the ash of the pre-ground plastic used in the feedstock is at least 30 wt.%, or at least 40 wt.%, or at least 50 wt.%, or at least 60 wt.%, or at least 70 wt.%, or at least 75 wt.%, based on the weight of the plastic ash. The upper limit is desirably not greater than 96 wt.%, or not greater than 90 wt.%, or not greater than 86 wt.%, based on the weight of the plastic ash.

[0088] In another embodiment, the amount of iron compounds in the ash of the pre-ground plastic used in the raw material is not greater than 20 wt.%, or not greater than 15 wt.%, or not greater than 10 wt.%, or not greater than 5 wt.%, or not greater than 3 wt.%, or not greater than 2 wt.%, or not greater than 1.5 wt.%, based on the weight of the plastic ash.

[0089] In another embodiment, the amount of aluminum compounds in the ash of the pre-ground plastic used in the raw material is not greater than 20 wt.%, or not greater than 15 wt.%, or not greater than 10 wt.%, or not greater than 5 wt.%, or not greater than 3 wt.%, or not greater than 2 wt.%, or not greater than 1.5 wt.%, based on the weight of the plastic ash.

[0090] In another embodiment, the amount of silicon compounds in the ash of the pre-ground plastic used in the raw material is not greater than 20 wt.%, or not greater than 15 wt.%, or not greater than 10 wt.%, or not greater than 8 wt.%, or not greater than 6 wt.%, based on the weight of the plastic ash.

[0091] Examples of plastics (i.e., organic synthetic polymers that are solid at 25 °C and 1 atmosphere) include acrylonitrile butadiene styrene (ABS), celluloses such as cellulose acetate, cellulose diacetate, cellulose triacetate, cellulose acetate propionate, cellulose acetate butyrate, and regenerated cellulose; epoxy resins, polyamides, phenolic resins, polyacetals, polycarbonates, polyesters, including PET (polyethylene terephthalate) and copolyesters, such as those containing residues of monomers TMCD (2,2,4,4-tetramethyl-1,3-cyclobutanediol), CHDM (cyclohexanedimethanol), propylene glycol, or NPG (neopentyl glycol); high density polyethylene, low density polyethylene, crosslinked polyethylene, polyphenyl alloy, polypropylene and its copolymers, other polyolefins, polystyrene, poly(methyl methacrylate), polytetrafluoroethylene, styrene-containing polymers, polyurethanes, vinyl polymers, styrene acrylonitrile, thermoplastic elastomers other than tires, which include thermoplastic elastomers, epoxy resins, and urea-containing polymers and melamine.

[0092] In one embodiment or in combination with any of the embodiments mentioned, the plastic feedstock comprises a thermosetting polymer. Examples of the amount of thermosetting polymer present in the plastic feedstock can be at least 5 wt.%, or at least 10 wt.%, or at least 15 wt.%, or at least 20 wt.%, or at least 25 wt.%, or at least 30 wt.%, or at least 40 wt.%, or at least 50 wt.%, or at least 60 wt.%, or at least 70 wt.%, or at least 80 wt.%, or at least 90 wt.%, or at least 95 wt.%, or at least 97 wt.%, or at least 98 wt.%, or 100 wt.%, based on the weight of all plastics in the feedstock or fed to the gasifier.

[0093] Examples of a series of articles containing one or more of the above polymers include packaging, engineering plastics, building and structural articles, household and domestic appliance articles, furniture, lawn and garden, and automotive plastics, which polymers can be size-reduced by granulation or shredding, or the compacted material can be first compacted and then size-reduced and fed into the gasifier. Examples of article types include bottles (for all types of applications such as beverages, food, detergents, cosmetics, personal care, etc.), bottle caps, cigarette filters and rods, spectacle frames, cups, lids, trays, plumbing pipes (such as PBT, PVC, and PEX pipes), cable insulation, sheets, tote bags, automotive moldings, bedding, seat cushions, seat covers, beverage machine fronts, fuel tanks, acrylic sheets, barrels, audio tapes, plumbing pipes, septic tanks, toys, food films, agricultural films, milk crate coatings, cable coatings, heavy industrial bags, sound insulation materials, helmets, surfboards, stretch films, industrial packaging films, thin-walled containers, crates and boxes, and industrial packaging materials and films, packaging made of spunbonded high-density polyethylene, such as for envelopes or medical packaging or house wrap materials, building insulation, diapers, sports equipment, spectacle lenses, CDs and DVDs, food packaging, microwave-safe containers, garden furniture, medical packaging and appliances, luggage, and kitchen utensils.

[0094] Any plastic used to prepare the gasifier feedstock can be formulated with the above additives and fillers, which additives and fillers include plasticizers, waxes, compatibilizers, biodegradation promoters, dyes, pigments, colorants, gloss control agents, lubricants, antioxidants, viscosity regulators, antifungal agents, antifogging agents, heat stabilizers, impact modifiers, flame retardants, corrosion inhibitors, antibacterial agents, softeners, fragrances, and mold release agents.

[0095] Any plastics used for preparing the raw materials of the gasifier can be formulated with additives and fillers, and the additives and fillers include plasticizers, waxes, compatibilizers, biodegradation promoters, dyes, pigments, colorants, gloss control agents, lubricants, antioxidants, viscosity regulators, antifungal agents, antifogging agents, heat stabilizers, impact modifiers, flame retardants, corrosion inhibitors, antibacterial agents, softeners, fragrances and mold release agents.

[0096] Plasticizers reduce the melting temperature, Tg and / or melt viscosity of the polymers used for preparing plastic products. Examples of plasticizers include phosphate plasticizers, benzoate plasticizers, adipate plasticizers, phthalate plasticizers, glycolates, citrate plasticizers and hydroxyl-functional plasticizers. More specifically, examples of plasticizers include triphenyl phosphate, tricresyl phosphate, tolyldiphenyl phosphate, octyldiphenyl phosphate, diphenyldiphenyl phosphate, trioctyl phosphate, tributyl phosphate, diethyl phthalate, dimethoxyethyl phthalate, dimethyl phthalate, dioctyl phthalate, dibutyl phthalate, bis(2-ethylhexyl) phthalate, butyl benzyl phthalate, dibenzyl phthalate, butyl phthalyl butyl glycolate, monoethylene glycol phthalate, butyl methyl phthalyl glycolate, triethyl citrate, tributyl citrate, triethyl acetyl citrate, tributyl acetyl citrate, tri(n-2-ethylhexyl) acetyl citrate, acetic acid glyceride (triacetin), diethylene glycol diacetate, triethylene glycol diacetate and tributyrin, diethylene glycol dibenzoate, rosin; hydrogenated rosin; stabilized rosin, and its mono-functional alcohol esters or polyol esters; modified rosin, including but not limited to maleic acid modified rosin and phenol modified rosin and their esters; terpene resin; phenol modified terpene resin; coumarin-indene resin; phenolic resin; alkylphenol-acetylene resin; and phenol-formaldehyde resin.

[0097] Some examples of plasticizers are those that are biodegradable. Examples of these plasticizers include acetic acid glyceride, triethyl citrate, triethyl acetyl citrate, polyethylene glycol, benzoate-containing plasticizers such as Benzoflex TM plasticizer series, poly(alkyl succinate) such as poly(butyl succinate), polyethersulfone, adipate-based plasticizers, soybean oil epoxide such as Paraplex TM plasticizer series, sucrose-based plasticizers, dibutyl sebacate, tributyrin, sucrose acetate isobutyrate, Resolflex TM plasticizer series, triphenyl phosphate, glycolate, 2,2,4-trimethyl-1,3-pentanediol diisobutyrate and polycaprolactone.

[0098] The amount of plasticizer in the polymer for manufacturing plastic products can be about 0.5 to about 50 weight percent, based on the weight of the polymer. Other ranges can be about 5 to about 35 weight percent, about 5 to about 30, and about 10 to about 20, based on the weight of the polymer.

[0099] Waxes are also used to increase hardness. See, for example, U.S. Patent 2,904,050, which is incorporated herein by reference.

[0100] The compatibilizer can be a non-reactive compatibilizer or a reactive compatibilizer. The compatibilizer can enhance the ability of the first polymer to achieve a desired small particle size to improve the dispersion of the first polymer in the second polymer, such as in an elastomer. The compatibilizer used can also improve the mechanical and physical properties of the elastomer composition by improving the interfacial interaction / adhesion between the first polymer and the elastomer or the second polymer.

[0101] The amount of compatibilizer in the polymer can be in the range of about 1 wt.% to about 40 wt.%, about 5 wt.% to about 20 wt.%, or about 10 wt.% to about 20 wt.%, based on the weight of the polymer.

[0102] If desired, biodegradation and decomposition agents, such as hydrolysis aids or any intentional degradation promoter additives, can be added to or incorporated in the polymer, added during or after the manufacture of the polymer, and melt or solvent mixed together. These additives can promote hydrolysis by releasing acidic or basic residues, and / or accelerate photo (UV) or oxidative degradation and / or promote the growth of selective microbial colonies to assist in decomposition and biodegradation in compost and soil media. In addition to promoting degradation, these additives can have additional functions, such as improving the processing properties of the product or improving mechanical properties.

[0103] A group of examples of decomposition agents includes inorganic carbonates, synthetic carbonates, nepheline syenite, talc, magnesium hydroxide, aluminum hydroxide, diatomaceous earth, natural or synthetic silica, calcined clay, etc. If used, it is desirable that these fillers be well dispersed in the polymer matrix. The fillers can be used alone, or in combination of two or more.

[0104] Another group of examples is aromatic ketones used as oxidative decomposition agents, including benzophenone, anthraquinone, anthrone, acetylbenzophenone, 4-octylbenzophenone, etc. These aromatic ketones can be used alone, or in combination of two or more.

[0105] Other examples include transition metal compounds used as oxidative decomposing agents, such as salts of cobalt or magnesium, preferably aliphatic carboxylic acid (C12-C20) salts of cobalt or magnesium, more preferably cobalt stearate, cobalt oleate, magnesium stearate and magnesium oleate; or anatase titanium dioxide, or titanium dioxide. Mixed-phase titanium dioxide particles can be used, in which both rutile and anatase crystal structures are present in the same particle. The photosensitizer particles can have a relatively high surface area, such as about 10 to about 300 square meters / g, or 20 to 200 square meters / g, measured by the BET surface area method. If desired, the photosensitizer can be added to a plasticizer. These transition metal compounds can be used alone or in combination of two or more.

[0106] Examples of rare earth compounds used as oxidative decomposing agents include rare earths belonging to Group 3A of the periodic table and their oxides. Specific examples thereof include cerium (Ce), yttrium (Y), neodymium (Nd), rare earth oxides, hydroxides, rare earth sulfates, rare earth nitrates, rare earth acetates, rare earth chlorides, rare earth carboxylates, etc. More specific examples include cerium oxide, cerium sulfate, ammonium ceric sulfate, ammonium cerium nitrate, cerium acetate, lanthanum nitrate, cerium chloride, cerium nitrate, cerium hydroxide, cerium octoate, lanthanum oxide, yttrium oxide, scandium oxide, etc. These rare earth compounds can be used alone or in combination of two or more.

[0107] Examples of basic additives used as oxidative decomposing agents include alkaline earth metal oxides, alkaline earth metal hydroxides, alkaline earth metal carbonates, alkali metal carbonates, alkali metal bicarbonates, ZnO and basic Al2O3. At least one basic additive can be MgO, Mg(OH)2, MgCO3, CaO, Ca(OH)2, CaCO3, NaHCO3, Na2CO3, K2CO3, ZnO, KHCO3 or basic Al2O3. In one aspect, alkaline earth metal oxides, ZnO and basic Al2O3 can be used as basic additives.

[0108] Examples of organic acid additives used as oxidative decomposing agents include acetic acid, propionic acid, butyric acid, valeric acid, citric acid, tartaric acid, oxalic acid, malic acid, benzoic acid, formates, acetates, propionates, butyrates, valeric acid, citrates, tartrates, oxalates, malates, maleic acid, maleates, phthalic acid, phthalates, benzoates and combinations thereof.

[0109] Examples of other hydrophilic polymers or biodegradation promoters can include diols, polyethers and polyols or other biodegradable polymers, such as poly(glycolic acid), poly(lactic acid), polydimethylsiloxane, polyoxalate, poly(α-ester), polycarbonate, polyanhydride, polyacetal, polycaprolactone, poly(orthoester), polyamino acid, aliphatic polyesters such as poly(butylene) succinate, poly(ethylene) succinate, starch, regenerated cellulose or aliphatic-aromatic polyesters such as PBAT.

[0110] The colorants may include carbon black, iron oxides such as red or blue iron oxide, titanium dioxide, silicon dioxide, cadmium red, calcium carbonate, kaolin, aluminum hydroxide, barium sulfate, zinc oxide, aluminum oxide; and organic pigments such as azo and bisazo and trisazo pigments, condensed azo, azo lakes, naphthol pigments, anthrapyrimidines, benzimidazolone, carbazole, diketopyrrolopyrrole, flavanthrone, indigo pigments, isoindolinone, isoindoline, isoanthrone violet, metal complex pigments, oxazine, perylene, violanthrone, perinone, pyrazoloquinazolone, quinophthalone, triarylmethonium pigments, triphenyl dioxazine, xanthene, thioindigo, indanthrone, isoindanthrone, anthrapyrimidine, anthraquinone, iso dibenzanthrone, triphenyl dioxazine, quinacridone and phthalocyanine series, especially copper phthalocyanine and its nuclear halogenated derivatives, as well as acid lakes, basic and mordant dyes, and isoindolinone pigments, and plant and vegetable dyes, and any other available colorants or dyes.

[0111] The gloss control agents and fillers for adjusting gloss include silicon dioxide, talc, clay, barium sulfate, barium carbonate, calcium sulfate, calcium carbonate, magnesium carbonate, etc.

[0112] Suitable flame retardants include silicon dioxide, metal oxides, phosphates, catechol phosphates, resorcinol phosphates, borates, inorganic hydrates and aromatic polyhalides.

[0113] The antifungal and / or antibacterial agents include polyene antifungals (e.g., natamycin, rimocidin, filipin, nystatin, amphotericin B, candicidin and hamycin), imidazole antifungals such as miconazole (available as obtained from WellSpring Pharmaceutical Corporation), ketoconazole (available as commercially available from McNeil Customer Healthcare), clotrimazole (available as and commercially available from Merck and as commercially available from Bayer), econazole, omoconazole, bifonazole, butoconazole, fenticonazole, isoconazole, oxiconazole, sertaconazole (available as obtained from Ortho Dermatologics), sulconazole and tioconazole; triazole antifungals such as fluconazole, itraconazole, isavuconazole, ravuconazole, posaconazole, voriconazole, terconazole and abafungin), thiazole antifungals (e.g., abafungin), allylamine antifungals (e.g., terbinafine (available as obtained from Novartis Consumer Health, Inc.), naftifine (available as Commercially available from Merz Pharmaceuticals) and butenafine (available as LOTRAMIN Commercially available from Merck), echinocandin antifungals (such as anidulafungin, caspofungin, and micafungin), polygonal dialdehyde, benzoic acid, ciclopirox olamine, tolnaftate (such as available as Commercially available from MDS Consumer Care, Inc.), undecylenic acid, flucytosine, 5-fluorocytosine, griseofulvin, iodochlorhydroxyquin, octanoic acid, and any combination thereof.

[0114] Viscosity regulators are used to regulate the melt flow index or viscosity of polymers and include polyethylene glycol and polypropylene glycol, as well as glycerol.

[0115] If desired, a fragrance can be added. Examples of fragrances include spices, spice extracts, herb extracts, essential oils, smelling salts, volatile organic compounds, volatile small molecules, methyl formate, methyl acetate, methyl butyrate, ethyl acetate, ethyl butyrate, isoamyl acetate, amyl butyrate, amyl valerate, octyl acetate, myrcene, geraniol, nerol, citral, citronellal, citronellol, linalool, nerolidol, limonene, camphor, terpineol, α-ionone, thujone, benzaldehyde, eugenol, isoeugenol, cinnamaldehyde, ethyl maltol, vanilla, vanillin, cinnamyl alcohol, anisole, anethole, estragole, thymol, carvacrol, furanone, methanol, rosemary, lavender, citrus, freesia, apricot blossom, green plants, peach, jasmine, rosewood, pine, thyme, oakmoss, musk, vetiver, myrrh, blackcurrant, bergamot, grapefruit, acacia, passionflower, sandalwood, tonka bean, citrus, neroli, violet leaf, gardenia, red fruits, ylang-ylang, acacia, mimosa, tonka bean, woods, ambergris, narcissus, hyacinth, narcissus, blackcurrant bud, iris, raspberry, lily of the valley, sandalwood, vetiver, cedar, neroli, strawberry, carnation, oregano, honey, civet, heliotrope, caramel, coumarin, patchouli, dewberry, helional, coriander, allspice, labdanum, cassie, aldehydes, orchid, amber, iris, tuberose, palmarosa, cinnamon, nutmeg, moss, benzoin, pineapple, foxglove, tulip, wisteria, clematis, ambergris, gum, resin, civet, plum, castoreum, civet, myrrh, geranium, rose mauve, kalanchoe, spicy carnation, galbanum, petitgrain, iris, honeysuckle, pepper, raspberry, benzoin, mango, coconut, limonene, castoreum, osmanthus, oakmoss, nectarine, mint, anise, cinnamon, iris grass, apricot, plumeria, marigold, rose essential oil, narcissus, tolu balsam, frankincense, amber, neroli, bourbon vetiver, centaurea, white musk, papaya, rock candy, jackfruit, honeydew, lotus, lily of the valley, mulberry, wormwood, ginger, juniper, mountain pepper, peony, violet, lemon, lime, hibiscus, white rum, basil, lavender, balsam, fo-ti-tieng, osmanthus, karokarunde), Michelia alba, Alocasia macrorrhiza, white rose, Lilium dauricum, marigold, ambergris, ivy, grass, gutta-percha, Dutch mint, sage, poplar, grape, bilberry (brimbelle), water lily, primrose, orchid, glycine, Tahitian gardenia, Hedychium coronarium, green osmanthus, passion flower, blue rose, laurel oil, acacia, African marigold, Anatolian rose, Auvergne narcissus, common broom, common broom chocolate, Bulgarian rose, Pogostemon cablin, Gardenia jasminoides Ellis, Calabrian citrus, tuberose, Ceylon cardamom, Caribbean passion fruit, Damask rose, Georgia peach, Madonna lily, Egyptian jasmine, Egyptian marigold, Ethiopian civet, Farnesian cassie, Phalaenopsis floribunda, French jasmine, French jonquil, French hyacinth, Guinea orange, Guyanese wacapua, Grasse petitgrain, Grasse rose, Grasse tuberose, Haitian vetiver, Hawaiian pineapple, Israeli basil, Indian sandalwood, Indian Ocean vanilla, Italian bergamot, Italian Phalaenopsis, Jamaican pepper, rose, ylang-ylang, Madagascar vanilla, Moroccan jasmine, Moroccan rose, Moroccan oakmoss, Moroccan neroli, Mysore sandalwood, Oriental rose, Russian leather, Russian coriander, Sicilian citrus, South African marigold, South American tonka bean, Singapore Pogostemon cablin, Spanish neroli, Sicilian lime, Reunion vetiver, Turkish rose, Thai benzoin, Tunisian neroli, Yugoslavian oakmoss, Virginia cedarwood, Utah yarrow, West Indian mahogany, etc. and any combination thereof. African marigold, Anatolian rose, Auvergne narcissus, common broom, common broom chocolate, Bulgarian rose, Pogostemon cablin, Gardenia jasminoides Ellis, Calabrian citrus, tuberose, Ceylon cardamom, Caribbean passion fruit, Damask rose, Georgia peach, Madonna lily, Egyptian jasmine, Egyptian marigold, Ethiopian civet, Farnesian cassie, Florence iris, French jasmine, French jonquil, French hyacinth, Guinea orange, Guyanese wacapua, Grasse petitgrain, Grasse rose, Grasse tuberose, Haitian vetiver, Hawaiian pineapple, Israeli basil, Indian sandalwood, Indian Ocean vanilla, Italian bergamot, Italian iris, Jamaican pepper, May rose, ylang-ylang, Madagascar vanilla, Moroccan jasmine, Moroccan rose, Moroccan oakmoss, Moroccan neroli, Mysore sandalwood, Oriental rose, Russian leather, Russian coriander, Sicilian citrus, South African marigold, South American tonka bean, Singapore Pogostemon cablin, Spanish neroli, Sicilian lime, Reunion vetiver, Turkish rose, Thai benzoin, Tunisian neroli, Yugoslavian oakmoss, Virginia cedar, Utah yarrow, West Indian padauk, etc., and any combination thereof.

[0116] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises a plastic, at least a part of which is obtained from cellulose, such as a cellulose derivative with an acyl substitution degree of less than 3 or from 1.8 to 2.8, such as cellulose acetate, diacetate cellulose, triacetate cellulose, cellulose acetate propionate, cellulose acetate butyrate.

[0117] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises a plastic, at least a part of which is obtained from a polymer having repeating terephthalate units, such as polyethylene terephthalate, polypropylene terephthalate, polybutylene terephthalate, and their copolyesters.

[0118] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises a plastic, at least a part of which is obtained from a copolyester having a plurality of cyclohexanedimethanol moieties, 2,2,4,4 - tetramethyl - 1,3 - cyclobutanediol moieties, or a combination thereof.

[0119] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises a plastic, at least a part of which is obtained from low - density polyethylene, high - density polyethylene, linear low - density polyethylene, polypropylene, polymethylpentene, polybutene - 1, and their copolymers.

[0120] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises a plastic, at least a part of which is obtained from high - density polyethylene or a fuel tank.

[0121] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises a plastic, at least a part of which is obtained from an eyeglass frame.

[0122] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises a plastic, at least a part of which is obtained from cross - linked polyethylene. Examples of the feedstock are those obtained from or including a cross - linked polyethylene pipe or its reduced - diameter portion. Cross - linked polyethylene is also commonly referred to as PEX. Its structure contains cross - links in the polymer, converting thermoplastic polyethylene into a polymer with stronger thermosetting properties. In one embodiment or in combination with any of the embodiments mentioned, cross - linked polyethylene is a thermosetting polymer. Cross - linked polyethylene can be obtained by cross - linking any polyethylene (LDPE, LLDPE, HDPE), but is typically obtained by cross - linking low - density polyethylene. The cross - linking method is not limited and can be done during and after the extrusion process. The degree of cross - linking can be at least 50%. In one embodiment or in combination with any of the embodiments mentioned, the degree of cross - linking meets ASTM F876. In one embodiment or in combination with any of the embodiments mentioned, the degree of cross - linking is from 60% to 92%, or from 65% to 89%.

[0123] The crosslinking method can be irradiating the tube with an electron beam. The Engel crosslinking method is to mix a peroxide with polyethylene, and crosslinking occurs before extrusion, such as in a long die. The crosslinking of polyethylene can also be accomplished in a silane- or vinylsilane-based method or in an azo-based method. The types of crosslinked polyethylene include PE-Xa (peroxide crosslinked, crosslinked at least 75%), PE-Xb (moisture cured or silane-based, crosslinked at least 65%), PE-Xc (electron beam-based, crosslinked at least 60%), and PE-Xd (azo-based, crosslinked at least 60%).

[0124] In one embodiment or in combination with any of the embodiments mentioned, the starting material comprises a plastic, at least a portion of which is obtained from plastic bottles.

[0125] In one embodiment or in combination with any of the embodiments mentioned, the starting material comprises a plastic, at least a portion of which is obtained from diapers.

[0126] In one embodiment or in combination with any of the embodiments mentioned, the starting material comprises a plastic, at least a portion of which is obtained from polystyrene foam or expanded polystyrene.

[0127] In one embodiment or in combination with any of the embodiments mentioned, the starting material comprises a plastic, at least a portion of which is obtained from spunbonded high-density polyethylene.

[0128] Suitable recycled plastics (i.e., organic synthetic polymers that are solid at 25 °C and 1 atmosphere of pressure) include those plastics having or classified with resin ID codes numbered 1 - 7 within the chasing arrow triangle established by SPI. In one embodiment or in combination with any of the embodiments mentioned, at least a portion of the feedstock for the gasifier, or at least a portion of the plastic recycle fed to the gasifier, comprises one or more plastics that are generally not recycled. These include plastics with the numbers 3 (polyvinyl chloride), 5 (polypropylene), 6 (polystyrene), and 7 (other). In one embodiment or in combination with any of the embodiments mentioned, the recycled plastics fed to the gasifier or at least a portion of the feedstock contain less than 10 wt.%, or no greater than 5 wt.%, or no greater than 3 wt.%, or no greater than 2 wt.%, or no greater than 1 wt.%, or no greater than 0.5 wt.%, or no greater than 0.2 wt.%, or no greater than 0.1 wt.%, or no greater than 0.05 wt.% of the plastic having or corresponding to identification number 3 (polyvinyl chloride), or optionally plastics having identification numbers 3 and 6, or optionally plastics having identification numbers 3, 6, and 7, based on the weight of all plastics fed to the gasifier or the gasification zone. In one embodiment or in combination with any of the embodiments mentioned, the recycled plastics fed to the gasifier or at least a portion of the feedstock comprise at least 1 wt.%, or at least 2 wt.%, or at least 3 wt.%, or at least 5 wt.%, or at least 7 wt.%, or at least 10 wt.%, or at least 12 wt.%, or at least 15 wt.%, or at least 20 wt.%, or at least 25 wt.%, or at least 30 wt.%, or at least 40 wt.%, or at least or greater than 50 wt.%, or at least 65 wt.%, or at least 85 wt.%, or at least 90 wt.% of the plastics having or corresponding to number 5, or number 6, or number 7, or a combination thereof, based on the weight of the plastics in the feed to the gasifier or the gasification zone or the feedstock. In one embodiment or in combination with any of the embodiments mentioned, the feed containing waste plastics can comprise at least 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, or 99 wt.% of at least one, two, three, or four different types of resin ID codes. In one embodiment or in combination with any of the embodiments mentioned, the feed containing waste plastics contains less than 25, 20, 15, 10, 5, or 1 wt.% of polyvinyl chloride.

[0129] One of the advantages of gasifying plastics is that many plastics that were landfilled because they could not be remelted (e.g., ground and melt - extruded into recycled products) can now be recycled and made into recycled products. An example of such a plastic is a thermoset plastic. In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises plastics at least a portion of which cannot be melt - extruded into recycled products.

[0130] One of the advantages of gasifying plastics is that many plastics cannot be recycled or mechanically recycled due to the presence of additives, coatings, or dyes / pigments, so they would be landfilled. Now these plastics can be recycled and made into recycled products. For example, some heavily dyed plastics, or plastics containing additives suitable for only a limited range of applications, or plastics with coatings, may impair the function or appearance of the recycled products. Other plastics are not usually mechanically recycled through the process in which plastics are melted because they are difficult to shred, granulate, or pulverize without first going through a compaction step, which increases the cost. These plastics that are not usually mechanically recycled have resin ID markings of 4, 5, 6, or 7 or a combination thereof.

[0131] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises plastics at least a portion of which cannot be recycled or mechanically recycled, optionally within a 10-mile radius of the gasifier, or within 50 miles, or within 100 miles, or within 150 miles, or within 200 miles, or within 250 miles, or within 300 miles, or within 400 miles, or within 500 miles, or within 600 miles, or within 700 miles, or within 800 miles, or within 1000 miles, or within 1250 miles, or within 1500 miles, or within a 2000-mile radius of the gasifier, or in the same province, state, or country as the location of the gasifier.

[0132] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises plastics at least a portion of which is obtained from polymers colored with pigments or dyes, optionally other than black.

[0133] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises plastics at least a portion of which is obtained from articles having a label layer where the article is reduced in diameter at the label.

[0134] In one embodiment or in combination with any of the embodiments mentioned, the feedstock comprises plastics at least a portion of which is obtained from articles that cannot be mechanically recycled due to the presence of additives in the articles.

[0135] The sources of post-consumer or post-industrial waste are not restricted. Post-consumer plastic sources can include plastics present in and / or separated from the municipal solid waste stream (“MSW”). For example, the MSW stream can be processed and sorted into several discrete components, including textiles, fibers, mixed plastics, paper, wood, glass, metal, etc. Other plastic sources include those obtained by collection agencies, or those obtained by or for or on behalf of plastic brand owners or alliances or organizations, or those obtained by brokers, or those obtained from post-industrial sources such as waste from mills or commercial production facilities, unsold fabrics from wholesalers or distributors, from mechanical and / or chemical sorting or separation facilities, from landfills, or stranded on docks or ships.

[0136] In one embodiment or in combination with any of the embodiments mentioned, at least a portion of the plastics in the feedstock, or the feedstock entering the gasifier or gasification zone, contains or is derived from cellulosic materials. Examples of cellulosic plastics include cellulose acetate, diacetate cellulose, triacetate cellulose, cellulose acetate propionate, cellulose acetate butyrate, regenerated cellulose such as viscose, rayon, and Lyocel TM products. These cellulosic articles can be in any form, such as films, sheets, molded or stamped products, and are included in or on any article. Examples of cellulosic articles that can be included in the feedstock or fed into the gasifier or gasification zone include ophthalmic products such as spectacle frames, tool handles such as screwdriver handles, optical films such as for displays or televisions, computers, mobile phones, photographic film, coatings, buttons, and toys, including building blocks. Desirably, the plastics contain low levels or no halogenated polymers, especially polyvinyl chloride, polyvinyl fluoride, polyvinylidene fluoride, and polytetrafluoroethylene, and other fluorinated or chlorinated polymers. The release of chlorine or fluorine elements or radicals over time can affect the life of the refractory lining on gasifiers operating at high temperatures and pressures. In one embodiment or in combination with any of the embodiments mentioned, the plastics contain less than 10 wt.%, or no more than 8 wt.%, or no more than 6 wt.%, or no more than 5 wt.%, or no more than 4 wt.%, or no more than 3.5 wt.%, or no more than 3 wt.%, or no more than 2.5 wt.%, or no more than 2 wt.%, or no more than 1.5 wt.%, or no more than 1 wt.%, or no more than 0.5 wt.%, or no more than 0.25 wt.%, or no more than 0.1 wt.%, or no more than 0.05 wt.%, or no more than 0.01 wt.% of halogenated polymers, based on the weight of the plastics. Desirably, the halides minimized or excluded are chlorine or fluorine.

[0137] Plastics used as co-fuels in a feedstock stream have the advantage that they do not require heat treatment before they are introduced into the gasification zone or before they are introduced into one or more components of the feedstock stream. Unlike wood or grain, which typically require heat treatment other than drying, such as drying in an oven, pre-ground plastics (those that are ground to their final size when combined into the feedstock stream) are not pyrolyzed or dried before being introduced into the gasifier, and desirably, the pre-ground plastics are not obtained from plastic sources that have already been pyrolyzed or dried. In another embodiment, the pre-ground plastics are not obtained from post-consumer plastics or post-industrial plastics that are melted or extruded after the consumption or industrial manufacturing stage, and desirably, the pre-ground plastics are not melted or extruded before they enter the gasifier. In another embodiment, post-consumer or post-industrial plastics, after shredding or any type of pelletizing, are not melted or extruded or subjected to heat treatment above their pyrolysis temperature, or above 150 °C, or above 110 °C, or above 100 °C, or above 90 °C, or above 80 °C, or above 60 °C, or above 58 °C, or above their nominal temperature, before they are introduced into the gasification zone. It should be noted that pre-ground plastics can be dried before they are introduced into the feedstock stream; however, this is not necessary in a slurry-based feedstock stream.

[0138] There is also provided a circular manufacturing method, comprising:

[0139] 1. providing recycled plastics, and

[0140] 2. reducing the diameter of the plastics to prepare pre-ground recycled plastics, and

[0141] 3. gasifying the pre-ground plastics to produce syngas derived from the recycled plastics, and

[0142] 4. or

[0143] (i) reacting the syngas derived from the recycled plastics to prepare recycled content intermediates, polymers, or articles (recycled PIA), each of which is at least partially derived from the syngas derived from the recycled plastics, or

[0144] (ii) allocating a recycled content allotment obtained from the recycled plastics or pre-ground plastics to intermediates, plastics, or polymers to produce recycled PIA; and

[0145] 5. optionally, sending at least a portion of the recycled PIA back as a feedstock to the gasification process step (i), or (ii), or (iii).

[0146] In the above method, a fully circular or closed-loop method is provided, in which plastics can be recycled multiple times to prepare plastics of the same family or class.

[0147] In this embodiment or in combination with any of the embodiments mentioned, a quota may be allocated to intermediates, plastics or polymers to directly produce recycled PIA from the recycled content value taken from the step of recycling plastics or pre - ground plastics or from the feedstock of gasifying a feedstock containing solid fossil fuels and recycled plastics or pre - ground plastics. Alternatively, a quota may be allocated to intermediates, plastics or polymers to indirectly produce recycled PIA by allocating the recycled content value taken from a recycling catalog, where the recycled content value is deposited into the recycling catalog from the recycled content present in the recycled plastics or pre - ground plastics, or from the recycled content value of the step of gasifying a feedstock containing solid fossil fuels and recycled plastics or pre - ground plastics.

[0148] In one embodiment, the recycled PIA is a plastic belonging to the same plastic family or category as the recycled plastic used in step (i).

[0149] In one embodiment, the recycled PIA can be prepared by a method in which the recycled plastics are gasified according to any of the methods described herein.

[0150] Also provided is a method for manufacturing a ring, comprising:

[0151] 1. A manufacturer of synthesis gas, or one of its entity families, or an entity contracted with any of them (collectively referred to as the "Recipient"), optionally and desirably receives recycled plastics (whether post - industrial or post - consumer) from industrial suppliers of the plastics or articles containing the plastics, and

[0152] 2. One or more Recipients reduce the size of the plastics (optionally, first compact the plastics, for example in the form of agglomerates or extrudates, and subsequently reduce the size or coarsely reduce the size / compact / further finely reduce the size) to prepare pre - ground recycled plastics, and

[0153] 3. One or more Recipients gasify the pre - ground plastics to produce synthesis gas derived from recycled plastics, and

[0154] 4. Or

[0155] (i) React the synthesis gas derived from the recycled plastics to prepare recycled content intermediates, polymers or articles (recycled PIA), each of which is at least partially derived from the synthesis gas derived from the recycled plastics, or

[0156] (ii) Allocate the recycled content quota obtained from the recycled plastics or the pre - ground plastics to intermediates, plastics or polymers to thereby produce recycled PIA; and

[0157] 5. Optionally, at least a portion of the recycled PIA is provided to the industrial supplier or to an entity contracted with the industrial supplier or with one of the industrial supplier's family of entities to supply the recycled PIA or articles made therefrom.

[0158] In this embodiment or in combination with any of the embodiments mentioned, a quota may be allocated to intermediates, plastics or polymers to directly produce recycled PIA from recycled content values taken from the step of recycling plastics or pre-ground plastics or from gasifying a feedstock containing solid fossil fuels and recycled plastics or pre-ground plastics, or a quota may be allocated to intermediates, plastics or polymers to indirectly produce recycled PIA by allocating recycled content values taken from a recycling catalog, where the recycled content values are deposited in the recycling catalog from the recycled content present in the recycled plastics or pre-ground plastics, or from the recycled content values from the step of gasifying a feedstock containing solid fossil fuels and recycled plastics or pre-ground plastics.

[0159] In the above method, a fully circular or closed-loop method is provided, in which plastics can be recycled multiple times to produce plastics of the same family or category. Industrial suppliers can provide plastics or plastic-containing articles to processor entities to process these plastics or articles into a form suitable or more suitable for gasification as further described herein to produce pre-ground plastics or precursors of pre-ground plastics, such as agglomerates, extrudates, fragments, etc., and the processor entity in turn supplies the pre-ground plastics or their precursors to a manufacturer of syngas or one of its entity families, and the manufacturer of syngas or its entity family can feed the pre-ground plastics as such into the feed stream of a gasifier, or can further process the precursor or pre-ground plastics into a final size suitable for gasification by any suitable method such as crushing or grinding. The gasification processes, equipment, and designs used can be any of those mentioned herein. The syngas produced using a feedstock containing pre-ground plastics can then be converted through a reaction scheme to produce recycled PIA, or the allotment generated from such a gasification step can be stored in a catalog of allotments, and from the catalog of allotments from any source, a portion thereof can be withdrawn and allocated to intermediates, polymers, or articles to produce recycled PIA. To close the circularity of plastics, at least a portion of the recycled PIA can be provided to the industrial supplier of the plastics or articles, or it can be provided to any entity contracted with the industrial supplier to process the recycled PIA into different forms, different sizes, or in combination with other components or plastics (e.g., a compounder and / or a sheet extruder), or to produce articles containing PIA to be provided to the industrial supplier or on behalf of the industrial supplier. The recycled PIA supplied to the industrial supplier or one of its contracted entities is desirably the same family or type of plastic as the plastics or plastic-containing articles supplied by the industrial supplier to the recipient.

[0160] "Recycle content allotment" or "allotment" means a recycle content value that:

[0161] a. is transferred from recycled waste (which is any recycled waste stream, whether or not it contains recycled plastics) to a receiving composition (e.g., a compound, polymer, article, intermediate, feedstock, product, or stream), and the receiving composition may or may not have physical components traceable to the recycled waste; or

[0162] b. is deposited into a recycle catalog, at least a portion of which is derived from recycled waste.

[0163] The recycle content value (whether by mass or percentage or any other unit of measurement) can optionally be determined according to a standard system used to trace, allocate, and / or credit recycle content in various compositions.

[0164] "Recycled content value" is a measure of the amount of material whose source is recycled plastic or pre-ground plastic. The recycled content value can be derived from any type of recycled plastic or any recycled plastic processed by any type of process prior to gasification.

[0165] The specific recycled content value can be determined by mass balance methods or mass ratios or percentages or any other unit of measure, and can be determined according to any system for tracing, allocating, and / or crediting recycled content in various compositions. The recycled content value can be deducted from the recycled inventory and applied to a product or composition to attribute the recycled content to the product or composition. The recycled content value does not have to be derived from gasified recycled plastic and can be a unit of measure with a known or unknown source in any technology used to process recycled plastic. In one embodiment, at least a portion of the recycled plastic from which a quota is obtained is also gasified as described in one or more of the embodiments throughout this document; for example, combined with a fossil fuel and gasified.

[0166] In one embodiment, at least a portion of the recycled content quota or recycled value deposited in the recycled content inventory is obtained from recycled plastic or pre-ground plastic. Desirably, at least 60%, or at least 70%, or at least 80%, or at least 90%, or at least 95%, or up to 100% of the following:

[0167] a. The quota, or

[0168] b. Deposited in the recycled inventory, or

[0169] c. The recycled content value in the recycled inventory, or

[0170] d. The recycled content value applied to a composition to produce recycled PIA

[0171] Is obtained from recycled plastic or pre-ground plastic.

[0172] The recycled content quota can include a recycled content quota or recycle content credit obtained through the transfer or use of raw materials. In one embodiment or in combination with any of the embodiments mentioned, the polymer, intermediate, composition, article, or stream receiving the recycled content quota can be or contain a portion of a non-recycled composition (e.g., a compound, polymer, feedstock, product, or stream). "Non-recycled" means a composition (e.g., a compound, polymer, feedstock, product, or stream) none of which is directly or indirectly derived from any type of recycled waste, including plastic.

[0173] "Recycled content allocation" and "allocation" refer to a type of recycled content quota where an entity or individual supplying a composition sells or transfers the composition to a receiving individual or entity, and the individual or entity preparing the composition has a quota, at least a portion of which can be associated with the composition sold or transferred by the supplying individual or entity to the receiving individual or entity. The supplying entity or individual can be controlled or owned by the same entity or individual or various affiliates that are ultimately at least partially controlled by a parent entity ("entity family"), or they can be from different entity families. Generally, the recycled content quota travels with the composition and its downstream derivatives. The allocation can be deposited into a recycling catalog and withdrawn from the recycling catalog as an allocation and applied to the composition to produce a recycled PIA.

[0174] "Recycled content credit" and "credit" refer to a type of recycled content quota where the quota can be used for sale or transfer or use, or has been sold or transferred or used, or:

[0175] a. does not sell the composition, or

[0176] b. sells or transfers the composition, but the quota is not associated with the sale or transfer of the composition, or

[0177] c. is deposited into or withdrawn from a recycling catalog that does not trace the molecules of the recycled content feedstock to the molecules of the resulting composition prepared with the recycled content feedstock, or the recycling catalog has such tracing ability but does not trace the specific quota applied to the composition.

[0178] In one embodiment or in combination with any of the embodiments mentioned, the allocation can be deposited into a recycling catalog, and the credit can be withdrawn from the catalog and applied to the composition to produce a recycled PIA. This would be the case where the allocation is generated from recycled plastic and deposited into the recycling catalog, the recycled content value is deducted from the recycling catalog and applied to the composition to produce a recycled PIA, which composition does not have a portion derived from syngas or does have a portion derived from syngas, but such syngas constituting that portion of the composition is not recycled content syngas. In this system, there is no need to trace the source of the reactant compound or composition back to the manufacture of the recycled-derived syngas stream or back to any atoms contained in the recycled-derived syngas stream, but rather any reactant compound or composition prepared by any method can be used and has been associated with such reactant compound or composition, or has been associated with a recycled PIA, a recycled content quota. In one embodiment, the recycled PIA reactant (the composition used to prepare the recycled PIA or the composition to which the quota is applied) does not contain recycled content.

[0179] In one embodiment, the composition receiving the quota for preparing recycled PIA is partially derived from a synthesis gas stream obtained by any gasification method. The feedstock for the gasification process may optionally include solid fossil fuels such as coal. The feedstock may also optionally include a combination of solid fossil fuels and recycled plastics or pre-ground plastics. In one embodiment, a method is provided, wherein:

[0180] a. Recycled plastics are obtained,

[0181] b. A recycled content value (or quota) is obtained from the recycled plastics, and

[0182] i. Deposited into a recycling catalog, and the quota (or score) is withdrawn from the recycling catalog and applied to the composition to obtain recycled PIA, or

[0183] ii. Applied to the composition to obtain recycled PIA; and

[0184] c. Optionally, according to any design or method described herein, optionally by combining at least a portion of the recycled plastics with solid fossil fuels as feedstock for the gasifier, subjecting it to a gasification process; and

[0185] d. Optionally, at least a portion of the composition in step b. is derived from a synthesis gas stream, optionally, the synthesis gas stream has been obtained by any feedstock and method described herein.

[0186] Steps b. and c. do not have to occur simultaneously. In one embodiment, they occur within one year of each other, or within six (6) months of each other, or within three (3) months of each other, or within one (1) month of each other, or within two (2) weeks of each other, or within one (1) week of each other, or within three (3) days of each other. The method allows for the passage of time between the moment a entity or individual receives the recycled plastics and generates a quota (which may occur after the receipt or ownership of the recycled plastics) and the actual processing of the recycled plastics in the gasifier.

[0187] As used herein, "recycle inventory" and "inventory" mean a group or set of quotas (allocations or credits) from which the deposit and deduction of quotas in any unit can be traced. The inventory can be in any form (electronic or paper), use any one or more software programs, or use various modules or applications that together trace deposits and deductions as a whole. Desirably, the total amount of recycled content taken out (or applied to the recycled PIA) is not greater than the total amount of recycled content quotas or credits deposited in the recycle inventory (from any source, not only from the gasification of recycled plastics). However, if a deficit in the recycled content value is achieved, the recycle content inventory is rebalanced to achieve a zero or positive available recycled content value. The timing of rebalancing can be determined and managed according to the rules of a specific certification system adopted by the recycled content syngas manufacturer or by one of its entity families, or alternatively, rebalanced within one (1) year, or six (6) months, or three (3) months, or one (1) month of achieving the deficit. The timing of depositing quotas into the recycle inventory, applying quotas (or credits) to a composition to produce recycled PIA, and gasifying recycled plastics need not be simultaneous or occur in any particular order. In one embodiment, the step of gasifying a specific volume of recycled plastics occurs after the recycled content value or quota from that volume of recycled plastics has been deposited into the recycle inventory. Additionally, the quota or recycled content value taken out of the recycle inventory need not be traceable to the recycled plastics or the gasified recycled plastics, but can be obtained from any waste recycle stream and any method of processing the recycle waste stream. Desirably, at least a portion of the recycled content value in the recycle inventory is obtained from recycled plastics, and optionally, at least a portion of the recycled plastics is processed in one or more gasification processes as described herein, optionally within one year of each other, and optionally, at least a portion of the volume of recycled plastics (from which the recycled content value was deposited into the recycle inventory) is also processed through any one or more of the gasification processes described herein.

[0188] Determining whether the recycled PIA is directly or indirectly derived from recycled waste is not based on the presence or absence of intermediate steps or entities in the supply chain, but on whether at least a portion of the recycled plastic molecules fed into the gasifier can be traced to the recycled PIA. If at least a portion of the molecules in the recycled PIA can optionally be traced through one or more intermediate steps or entities to at least a portion of the recycled content syngas molecules, then the recycled PIA is considered to be directly derived from or in direct contact with the recycled plastics. Any number of intermediates and intermediate derivatives can be prepared before producing the recycled PIA.

[0189] Recycled PIA can be indirectly derived from recycled plastics if no part of its molecule is obtained from recycled-content syngas molecules, or if some parts of its molecule are obtained from recycled-content syngas molecules, but the recycled PIA has a recycled-content value exceeding that associated with the recycled-content syngas molecules, and in the latter case, the recycled PIA can be directly and indirectly derived from recycled plastics.

[0190] In one embodiment or in combination with any of the embodiments mentioned, the recycled PIA is indirectly derived from recycled plastics or recycled-content syngas. In another embodiment, the recycled PIA is directly derived from recycled plastics or recycled-content syngas. In another embodiment, the recycled PIA is indirectly derived from recycled plastics or recycled-content syngas, and no part of the recycled PIA is directly derived from recycled plastics or recycled-content syngas.

[0191] In another embodiment, various methods are provided for allocating recycled content among various recycled PIA compositions, the various recycled PIA compositions being made by any one entity or combination of entities in a family of entities of which the recycled-content syngas manufacturer is a part. For example, the recycled-content syngas manufacturer, or any combination or all of its family of entities, or a site, may:

[0192] a. Adopt a symmetric distribution of recycled-content values in its products based on the same fractional percentage of recycled content in one or more feedstocks or based on the quota amount received. For example, if 5 wt.% of the gasification feedstock is recycled plastics, or if the recycled-content value is 5 wt.% of all the gasification feedstock, then all the recycled PIA compositions can contain 5 wt.% of the recycled-content value. In this case, the amount of recycled content in the product is proportional to the amount of recycled content in the feedstock used to prepare the product; or

[0193] b. Employ an asymmetric distribution of recycled content values in its products based on the same fractional percentage of recycled content in one or more feedstocks or based on the received quota amount. For example, if 5 wt.% of the gasifier feed is recycled plastic, or if the quota value is 5 wt.% of the entire gasifier feed, then one volume or batch of recycled PIA can receive a greater amount of recycled content value than other batches or volumes of recycled PIA. One batch of PVA can contain 20 mass% of recycled content, while another batch can contain 0% of recycled content, even if the two volumes can be identical in composition, as long as the amount of recycled content value taken from the recycling inventory and applied to the recycled PIA does not exceed the amount of recycled content value deposited in the recycling inventory, or if a deficit is achieved, the overdraft is rebalanced to zero or a positive scoring available state as described above. In the asymmetric distribution of recycled content, the manufacturer can customize the recycled content to the volume of recycled PIA sold among customers as needed, thus providing flexibility among customers, some of whom may require more recycled content in the volume of PVA than others.

[0194] The symmetric and asymmetric distributions of recycled content can be proportional on a site-wide basis or on a multi-site basis. In one embodiment or in combination with any of the embodiments mentioned, the recycled content input (recycled plastic or quota) can be within a site, and the recycled content value from said input is applied to one or more compositions prepared at the same site to prepare recycled PIA. The recycled content value can be applied symmetrically or asymmetrically to one or more different compositions prepared at the site.

[0195] In one embodiment or in combination with any of the embodiments mentioned, the recycled content input or generation (recycled content feedstock or quota) can be to or at a first site, and the recycled content value from said input is transferred to a second site and applied to one or more compositions prepared at the second site. The recycled content value can be applied symmetrically or asymmetrically to the compositions at the second site.

[0196] As used herein, a compound or composition includes liquids, solids, formulations, polymers, and each of the solids can be in any form, including pellets, sheets, films, strands, pads, meshes, fibers, flakes, extrudates, agglomerates, etc.

[0197] In one embodiment, the recycled PIA has an amount of recycled content associated with it, or contained in it, or labeled, advertised or certified as containing, of at least 0.01 wt.%, or at least 0.05 wt.%, or at least 0.1 wt.%, or at least 0.5 wt.%, or at least 0.75 wt.%, or at least 1 wt.%, or at least 1.25 wt.%, or at least 1.5 wt.%, or at least 1.75 wt.%, or at least 2 wt.%, or at least 2.25 wt.%, or at least 2.5 wt.%, or at least 2.75 wt.%, or at least 3 wt.%, or at least 3.5 wt.%, or at least 4 wt.%, or at least 4.5 wt.%, or at least 5 wt.%, or at least 6 wt.%, or at least 7 wt.%, or at least 10 wt.%, or at least 15 wt.%, or at least 20 wt.%, or at least 25 wt.%, or at least 30 wt.%, or at least 35 wt.%, or at least 40 wt.%, or at least 45 wt.%, or at least 50 wt.%, or at least 55 wt.%, or at least 60 wt.%, or at least 65 wt.%; and / or the amount can be at most 100 wt.%, or at most 95 wt.%, or at most 90 wt.%, or at most 80 wt.%, or at most 70 wt.%, or at most 60 wt.%, or at most 50 wt.%, or at most 40 wt.%, or at most 30 wt.%, or at most 25 wt.%, or at most 22 wt.%, or at most 20 wt.%, or at most 18 wt.%, or at most 16 wt.%, or at most 15 wt.%, or at most 14 wt.%, or at most 13 wt.%, or at most 11 wt.%, or at most 10 wt.%, or at most 8 wt.%, or at most 6 wt.%, or at most 5 wt.%, or at most 4 wt.%, or at most 3 wt.%, or at most 2 wt.%, or at most 1 wt.%, or at most 0.9 wt.%, or at most 0.8 wt.%, or at most 0.7 wt.%. The recycled content associated with the recycled PIA can be associated by applying a quota (scoring or allocation) to any polymer and / or article manufactured or sold. The quota can be included in a quota catalog created, maintained or operated by or for the recycled PIA manufacturer. The quota can be obtained from any source along any manufacturing chain of the product, provided its source is in the gasification of a feedstock containing solid fossil fuels and pre-ground plastics.

[0198] The amount of recycled content in the reactant compound or composition, or the amount of recycled content applied to the recycled PIA, or, in the case where all the recycled content from the recycled plastic feedstock is applied to the recycled PIA, the amount of recycled plastic (recycled plastic feedstock) required to feed the gasifier to achieve the required amount of recycled content in the recycled PIA, can be determined or calculated by any of the following methods:

[0199] (i) The quota amount associated with the recycled PIA is determined by the amount certified or declared by the supplier of the transferred recycled PIA, or

[0200] (ii) the allocated amount declared by the entity using the recycled PIA, or

[0201] (iii) using the mass balance method, back-calculate the minimum amount of recycled content in the raw material from the amount of recycled content declared, advertised or responsible for by the manufacturer, whether accurate or not, as applied to recycled PIA products,

[0202] (iv) using the proportional mass method to blend non-recycled content with pre-ground plastic raw materials, or associate the recycled content with a portion of the raw material.

[0203] In one embodiment, the recycled PIA manufacturer may prepare recycled PIA, or process reactant compounds or compositions and prepare recycled PIA, or prepare recycled PIA by obtaining reactant compounds or compositions from any source from a supplier, whether or not such reactant compounds or compositions have any recycled content, and:

[0204] i. From the same supplier of the reactant compound or composition, also obtain the recycled content quota applied to syngas or applied to any product, article, polymer or composition, or

[0205] ii. Obtain the recycled content quota from any individual or entity without the individual or entity transferring the recycled content quota providing the reactant compound or composition.

[0206] (i) The quota in (i) can be obtained from the supplier of the reactant compound or composition used to prepare the recycled PIA, and the supplier also supplies and transfers the reactant compound or composition to the recycled PIA manufacturer or its entity family. The situation described in (i) allows the recycled PIA manufacturer to obtain the supply of the reactant compound or composition with non-recycled content and also obtain the recycled content quota from the reactant compound or composition. In one embodiment, the reactant compound or composition supplier transfers the recycled content quota to the recycled PIA manufacturer and transfers the supply of the reactant compound or composition to the recycled PIA manufacturer, where the recycled content share is not associated with the supplied reactant compound or composition, provided that the transferred recycled content share is derived from the gasification of recycled pre-ground plastics. The recycled content quota does not have to be associated with the amount of recycled content in the reactant compound or composition or any monomer used to prepare the recycled PIA, but the recycled content quota transferred by the reactant compound or composition supplier can be related to other products in the recycled-derived synthesis gas stream from which it originated, rather than to products in the reaction process for preparing the polymer and / or article. For example, the reactant compound or composition can transfer the recycled content associated with r-butyraldehyde to the recycled PIA manufacturer and can also provide a certain amount of propionic anhydride, even if r-butyraldehyde is not directly or via downstream products used in the synthesis of polymers and / or articles such as cellulose diacetate. This allows for flexibility in allocating the recycled content between the reactant compound or composition supplier and the recycled PIA manufacturer among the various products they each manufacture. However, in each of these cases, the recycled content quota originates from the gasification of recycled plastics.

[0207] In one embodiment, the reactant compound or composition supplier transfers the recycled content quota to the recycled PIA manufacturer and transfers the supply of the reactant compound or composition to the recycled PIA manufacturer, where the recycled content quota is associated with the reactant compound or composition. Optionally, the supplied reactant compound or composition can be derived from recycled plastic feedstock, and at least a portion of the transferred recycled content quota can be the recycled content in the reactant compound or composition. The recycled content quota transferred to the recycled PIA manufacturer can be before the supply of the reactant compound or composition, optionally in batches, or together with each partial supplier of the reactant compound or composition, or allocated among the parties as needed.

[0208] (ii) The allocation in (ii) is obtained by the recycled PIA manufacturer (or its family of entities) from any individual or entity without obtaining a supply of reactant compounds or compositions from that individual or entity. The individual or entity may be a reactant compound or composition manufacturer that does not supply reactant compounds or compositions to the recycled PIA manufacturer or its family of entities, or the individual or entity may be a manufacturer that does not manufacture reactant compounds or compositions. In either case, the situation in (ii) allows the recycled PIA manufacturer to obtain a recycled content quota without having to purchase any reactant compounds or compositions from the entity supplying the recycled content quota. For example, an individual or entity may transfer the recycled content quota to the recycled PIA manufacturer or its family of entities through a buy / sell mode or contract without the need to purchase or sell the quota (e.g., as an exchange of products that are not reactant compounds or compositions), or the individual or entity may directly sell the quota to one of the recycled PIA manufacturer or its family of entities. Alternatively, the individual or entity may transfer a product other than reactant compounds or compositions together with its associated recycled content quota to the recycled PIA manufacturer. This is attractive for a recycled PIA manufacturer with a diverse business that manufactures various products other than recycled PIA, and the raw materials required for these products are not reactant compounds or compositions that an individual or entity can supply to the recycled PIA manufacturer.

[0209] Quotas may be deposited into a recycling directory (e.g., a quota directory). In one embodiment, the quota is an allocation created by a manufacturer of a recycled-derived synthesis gas stream. The recycled PIA manufacturer may also manufacture polymers and / or articles and withdraw from the directory whether or not recycled content is applied to the polymers and / or articles and whether or not recycled content is used for the polymers and / or articles. For example, the manufacturer of the recycled-derived synthesis gas stream and / or the recycled PIA manufacturer may:

[0210] a. Deposit the quota into the directory and only store it; or

[0211] b. Deposit the quota into the directory and apply the quota from the directory to products other than:

[0212] i. Any product directly or indirectly derived from the recycled-derived synthesis gas stream, or

[0213] ii. Polymers and / or articles prepared by the recycled PIA manufacturer, or

[0214] c. Sell or transfer the quota from the directory, with at least one quota obtained as described above deposited into the directory.

[0215] However, if desired, any amount of any recycled content quota can be deducted from the directory and applied to the polymer and / or article to produce recycled PIA. For example, a recycled directory can be generated with quotas having various sources for creating the quotas. Some recycled content quotas (scores) can be derived from the methanolysis of recycled waste, or from mechanical recycling of waste plastics or metals, and / or from pyrolysis of recycled waste, or from any other chemical or mechanical recycling technique. The recycled directory can track or not track the source or basis for obtaining the recycled content value, or the directory can not allow the associated source or basis of the allocation to be associated with the allocation applied to the recycled PIA. As long as the allocation is deducted from the allocation directory and applied to the recycled PIA regardless of the source of the allocation is sufficient, as long as the recycled content quota obtained from the recycled plastic feedstock containing solid fossil fuels and pre-ground plastics exists in the quota directory at the time of removal, or the recycled PIA manufacturer obtains the recycled content quota as specified in step (i) or step (ii), regardless of whether the recycled content quota is actually deposited in the directory. In one embodiment, the recycled content quota obtained in step (i) or (ii) is deposited in the quota directory. In one embodiment, the recycled content quota deducted from the directory and applied to the recycled PIA is derived from the gasification of a recycled plastic feedstock containing solid fossil fuels and pre-ground plastics.

[0216] As used throughout, the quota directory can be owned by the recycled syngas manufacturer, or by the recycled PIA manufacturer, or operated by either of them, or not owned or operated by either, but at least in part for the benefit of either of them, or licensed by either of them. Similarly, as used throughout, the recycled syngas manufacturer or the recycled PIA manufacturer can also include any one of their entity families. For example, although any one of them may not own or operate the directory, one of their entity families can own such a platform, or license it from an independent provider, or operate it for any one of them. Alternatively, an independent entity can own and / or operate the directory and operate and / or manage at least a portion of the directory for a service fee for any one of them.

[0217] In one embodiment, the recycled PIA manufacturer obtains a supply of reactant compounds or compositions from a supplier and also obtains a quota from the supplier, where such quota amount is derived from the gasification of a feedstock containing solid fossil fuels and pre-ground plastics, and optionally the quota is associated with the supplied reactant compounds or compositions. In one embodiment, at least a portion of the quota obtained by the recycled PIA producer is:

[0218] a. Applied to the recycled PIA prepared from the supply of reactant compounds or compositions;

[0219] b. Applied to recycled PIA that is not prepared from the supply of reactant compounds or compositions, such as in cases where recycled PIA has already been prepared and stored in a catalog or will be prepared in the future; or

[0220] c. Deposited into a catalog, from which the quota applied to recycled PIA (recycled PIA application allocation) is deducted, and the deposited allocation contributes or does not contribute to the amount of recycled PIA application allocation withdrawn therefrom.

[0221] d. Deposited into a catalog and stored.

[0222] In all embodiments, it is not necessary to use recycled plastic feedstock to prepare recycled PIA compositions, or to obtain recycled PIA from the recycled content quota associated with reactant compounds or compositions. Additionally, it is not necessary to apply the quota to recycled plastic feedstock to prepare recycled PIA, and the recycled content is applied to this recycled PIA. Instead, as described above, even if associated with reactant compounds or compositions when obtaining them, the quota can be deposited into an electronic catalog. However, in one embodiment, the reactant compounds or compositions associated with the quota are used to prepare recycled PIA compounds or compositions. In one embodiment, recycled PIA is obtained from the recycled content quota associated with gasified recycled plastic feedstock. In one embodiment, at least a portion of the quota obtained from gasifying solid fossil fuels and pre-ground plastics is applied to recycled PIA to prepare recycled PIA.

[0223] In one embodiment, a recycled-derived synthesis gas stream manufacturer generates a quota by gasifying a combination of solid fossil fuels and pre-ground plastics, and:

[0224] a. Applies the quota to any compound or composition (whether liquid or solid or any form of polymer, including pellets, sheets, fibers, flakes, etc.) prepared directly or indirectly (e.g., through a reaction scheme of several intermediates) from the recycled-derived synthesis gas stream; or

[0225] b. Applies the quota to compounds or compositions that are not prepared directly or indirectly from the recycled-derived synthesis gas stream, such as in the case of reactant compounds or compositions that have already been prepared and stored in a catalog or non-recycled content reactant compounds or compositions to be prepared in the future; or

[0226] c. Deposits it into a catalog, from which any allocation applied to reactant compounds or compositions is deducted; and the deposited allocation is associated or not associated with a specific allocation applied to reactant compounds or compositions; or

[0227] d. Is deposited into a catalog and stored for future use.

[0228] Also provided are packages or combinations that recycle PIA and recycle content identifiers associated with the recycled PIA, where the identifier is or includes an indication that the recycled PIA contains or is derived from or associated with recycled content. The package can be any suitable package for containing polymers and / or articles, such as plastic or metal drums, railroad cars, isotainers, totes, polytotes, IBC totes, bottles, compressed bales, oil drums, and plastic bags. The identifier can be a certificate document, a product specification stating the recycled content, a label, a logo or certification mark from a certifying agency, which indicates that the article or package contains the content or the recycled PIA contains the content, or is made from the source or associated with the recycled content, or it can be an electronic statement accompanied by the recycled PIA manufacturer with the purchase order or product, or posted as a statement, display on a website, or a logo indicating that the recycled PIA contains or is made from a source associated with or containing the recycled content, or it can be an electronically transmitted advertisement associated with the recycled PIA in each case by a website or in a website, by email, or by television or through a trade show. The identifier does not need to state or indicate that the recycled content is obtained from gasifying a feedstock containing solid fossil fuels and pre-ground plastics. Instead, the identifier can simply convey or communicate that the recycled PIA has or is derived from recycled content, regardless of the source. However, the recycled PIA has a recycled content quota that is at least partially derived from gasifying solid fossil fuels and recycled plastics.

[0229] In one embodiment, recycled content information about the recycled PIA can be communicated to a third party, where such recycled content information is based on or derived from at least a portion of an allocation or score. The third party can be a recycled syngas manufacturer or a customer of the recycled PIA manufacturer or supplier, or can be any other individual or entity or government organization other than the entity owning any of them. The transmission can be electronic, via a document, via an advertisement, or any other means of communication.

[0230] In one embodiment, a system or package is provided that includes:

[0231] a. Recycled PIA or an article made therefrom, and

[0232] b. An identifier associated with the recycled PIA or an article made therefrom, such as a score, label, or certificate, where the identifier is an indication that the polymer and / or article or an article made therefrom has or is derived from recycled content

[0233] Provided that the recycled PIA or an article made therefrom has a quota, or is made from a reactant compound or composition that is at least partially directly or indirectly derived from gasifying solid fossil fuels and pre-ground recycled plastics.

[0234] The system can be a physical combination, such as a package that at least has recycled PIA as its content, and the package has a label, such as an identifier, that is, for example, the content of the recycled PIA has or is derived from recycled content. Alternatively, whenever it transfers or sells recycled PIA that has or is derived from recycled content, a label or certificate can be issued to a third party or customer as part of the entity's standard operating procedure. The identifier does not have to be physically on the recycled PIA or the package, and does not have to be on any physical document accompanying or associated with the recycled PIA. For example, the identifier can be an electronic score transmitted by the recycled PIA manufacturer to the customer related to the sale or transfer of the recycled PIA product, and only because it is a score, it represents that the recycled PIA has recycled content. The identifier itself only needs to convey or communicate that the recycled PIA has or is derived from recycled content, regardless of the source. In one embodiment, an article made from recycled PIA can have an identifier, such as a stamp or logo embedded or adhered to the article. In one embodiment, the identifier is an electronic recycled content score from any source. In one embodiment, the identifier is an electronic recycled content score that is derived from gasifying a feedstock containing solid fossil fuels and pre-ground plastics.

[0235] Recycled PIA is made from reactant compounds or compositions, whether or not the reactants are recycled content reactants (recycled plastic feedstock). Once the recycled PIA composition is prepared, it can be designated as having recycled content based on and derived from at least a portion of a quota, again, regardless of whether recycled plastic feedstock was used to prepare the recycled PIA composition. The allocation can be taken or deducted from a catalog. The amount deducted and / or applied to the recycled PIA can correspond to any of the above methods, such as the mass balance method.

[0236] In one embodiment, the recycled PIA compound or composition can be prepared by having an allocation catalog, reacting the reactant compound or composition with a synthesis method to produce the recycled PIA, and applying the recycled content to the recycled PIA, thereby obtaining the recycled PIA by deducting the allocated amount from the allocation catalog. The recycled PIA manufacturer can have an allocation catalog that is owned by itself or by one entity in a family of entities that own, handle, or operate the catalog, or by a third party that operates at least a portion of the catalog for the recycled PIA manufacturer or its family of entities, or as a service provided to one entity in the recycled PIA manufacturer or its family of entities. The allocated amount deducted from the catalog is flexible and will depend on the amount of recycled content applied to the recycled PIA. It is sufficient to correspond to at least a portion, if not the complete amount, of the recycled content applied to the recycled PIA. The calculation method can be a mass balance method or the above-mentioned calculation method. The allocation catalog can be established on any basis and can be a mixture of bases, as long as at least a certain amount of the allocations in the catalog can be attributed to the gasification of a feedstock containing solid fossil fuels and pre-ground plastics. The recycled content quota applied to the recycled PIA does not have to be sourced from the gasification of a feedstock containing solid fossil fuels and pre-ground plastics, but can be sourced from any other method of generating allocations from recycled waste, such as by methanolysis or gasification of recycled waste, provided that the quota catalog also contains a quota or has a quota deposited, the source of which is the gasification of a feedstock containing solid fossil fuels and pre-ground plastics. However, in one embodiment, the recycled content applied to the recycled PIA is the quota obtained by gasifying a feedstock containing solid fossil fuels and pre-ground plastics.

[0237] Examples of recycled content designated or declared to the recycled PIA or to the reactant compound or composition are as follows:

[0238] 1. The recycled PIA manufacturer applies at least a portion of the quota to a polymer and / or article composition, where the share is associated with a synthesis gas stream derived from pre-ground plastics, and the reactant compound or composition used to prepare the recycled PIA does not contain any recycled content or it does contain recycled content; or

[0239] 2. The recycled PIA manufacturer applies at least a portion of the quota to a polymer and / or article composition, where the share is directly or indirectly obtained from a recycled content reactant compound or composition, regardless of whether such reactant compound or composition volume is used to manufacture the recycled PIA; or

[0240] 3. The recycled PIA manufacturer applies at least a portion of the quota to a recycled PIA composition, where the quota is directly or indirectly derived from recycled plastic feedstock used to manufacture the recycled PIA to which the quota is applied, and:

[0241] a. Apply all the recycled content in the recycled plastic feedstock to determine the amount of recycled content in the recycled PIA, or

[0242] b. Only a portion of the recycled content in the recycled plastic feedstock is applied to determine the amount of recycled content applied to the recycled PIA, and the remaining portion stored in the inventory is used for future recycled PIA, or for other existing recycled PIA made from recycled plastic feedstock without any recycled content, or for increasing the recycled content on existing recycled PIA, or a combination thereof, or

[0243] c. The recycled content in the recycled plastic feedstock is not applied to the recycled PIA but is stored in the inventory, and the recycled content from any source is deducted from the inventory and applied to the recycled PIA; or

[0244] 4. The recycled PIA manufacturer applies at least a portion of the quota to the reactant compound or composition used to manufacture the recycled PIA, thereby obtaining the recycled PIA, where the quota is obtained by transferring or purchasing the same reactant compound or composition used to manufacture the recycled PIA, and the quota is associated with the recycled content in the reactant compound or composition; or

[0245] 5. The recycled PIA manufacturer applies at least a portion of the quota to the reactant compound or composition used to manufacture the recycled PIA, thereby obtaining the recycled PIA, where the quota is obtained by transferring or purchasing the same reactant compound or composition used to manufacture the recycled PIA, and the quota is not associated with the recycled content in the reactant compound or composition; rather, it is associated with the recycled content of the monomers used to manufacture the reactant compound or composition; or

[0246] 6. The recycled PIA manufacturer applies at least a portion of the quota to the reactant compound or composition used to manufacture the recycled PIA, thereby obtaining the recycled PIA, where the quota is not obtained by transferring or purchasing the reactant compound or composition, and the quota is associated with the recycled content in the reactant compound or composition; or

[0247] 7. The recycled PIA manufacturer applies at least a portion of the quota to the reactant compound or composition used to manufacture the recycled PIA, thereby obtaining the recycled PIA, where the quota is not obtained by transferring or purchasing the same reactant compound or composition, and the quota is not associated with the recycled content in the reactant compound or composition; rather, it is associated with the recycled content of any monomers used to manufacture the reactant compound or composition; or

[0248] 8. The recycled PIA manufacturer obtains an allocation that is sourced from gasifying a feedstock containing solid fossil fuel and pre - ground plastic, and:

[0249] a. Do not apply a portion of the quota to the reactant compound or composition to prepare recycled PIA, and apply at least a portion to recycled PIA to prepare recycled PIA; or

[0250] b. Less than the entire portion is applied to the reactant compound or composition for preparing recycled PIA, and the remaining portion is stored in a catalog or applied to recycled PIA to be prepared in the future or to existing recycled PIA in the catalog.

[0251] In one embodiment, recycled PIA or an article prepared therefrom may be offered for sale or sold as recycled PIA containing recycled content or obtained with recycled content. The offer for sale or sale may be accompanied by a recycled content claim associated with the recycled PIA or a certification or representation of the article made with the recycled PIA.

[0252] The acquisition of the allocation and designation (whether internally, e.g., through a bookkeeping or catalog-tracking software program, or externally, through declarations, certifications, advertisements, representations, etc.) may be by the recycled PIA manufacturer or within the recycled PIA manufacturer entity family. Designating at least a portion of the recycled PIA as corresponding to at least a portion of the quota (e.g., allocating or scoring) may be done in various ways and according to the system employed by the recycled PIA manufacturer, which may vary by manufacturer. For example, the designation may occur internally simply through a log entry in the books or files of the recycled PIA manufacturer or other catalog software program, or through a specification, packaging, advertisement or declaration on the product, through a logo associated with the product, through a certification declaration associated with the product being sold, or through a formula that calculates the amount deducted from the catalog relative to the amount of recycled content applied to the product.

[0253] Optionally, recycled PIA may be sold. In one embodiment, a method of offering for sale or selling a polymer and / or article is provided by:

[0254] a. A recycled PIA manufacturer or its entity family, which obtains or generates a recycled content allocation, and the allocation may be obtained by any of the methods described herein and deposited into a catalog, the source of the recycled content allocation being the gasification of a feedstock containing solid fossil fuel and pre-ground plastic,

[0255] b. Transforming a reactant compound or composition during a synthesis process to prepare a compound, composition, polymer, and / or article composition,

[0256] c. Designate (e.g., allocate or associate) the recycled content from the allocation directory to at least a portion of the compound, composition, polymer, and / or article composition, where the directory contains at least one entry that is an allocation resulting from the gasification of a feedstock containing pre-ground plastic. The designation can be the amount of allocation deducted from the directory or the amount of recycled content declared or determined by the recycled PIA manufacturer in its account. Thus, the amount of recycled content does not necessarily have to be physically applied to the recycled PIA product. The designation can be an internal designation by or for the recycled PIA manufacturer or its entity family or a service provider having a contractual relationship with the recycled PIA manufacturer or its entity family, and

[0257] d. Offer for sale or sell a compound, composition, polymer, and / or article composition containing or obtained from at least a portion of the recycled content corresponding to the designation. The amount of recycled content represented as being included in the recycled PIA sold or offered for sale is related or associated with the designation. The amount of recycled content can be a 1:1 relationship between the amount of recycled content declared on the recycled PIA sold or offered for sale and the amount of recycled content allocated or designated by the recycled PIA manufacturer to the recycled PIA.

[0258] The steps need not be sequential and can be independent of each other. For example, if a recycled plastic feedstock composition is used to prepare the recycled PIA, the step a) of obtaining the allocation and the step of preparing the recycled PIA from the reactant compound or composition can be simultaneous and related because the recycled plastic feedstock is both the reactant compound or composition and has an associated recycled content allocation.

[0259] As used throughout, the step of deducting the allocation from the allocation directory does not require its application to the recycled PIA product. The deduction also does not mean that the quantity disappears or is removed from the directory log. The deduction can be an adjustment of the entry, removal, addition of an entry as a debit, or any other algorithm for adjusting the input and output based on the amount of recycled content associated with the product and one or the cumulative deposited allocation amounts in the directory. For example, the deduction can be a simple step of deducting / debiting an entry from one column and adding / crediting to another column within the same program or ledger, or an automated deduction and entry / addition and / or application or designation to the product information board algorithm. The step of applying the allocation to the recycled PIA product (where such an allocation is deducted from the directory) also does not require the physical application of the allocation to the recycled PIA product or any document issued in connection with the recycled PIA product sold. For example, the recycled PIA manufacturer can ship the recycled PIA product to a customer and satisfy the "application" of the allocation for the recycled PIA product by electronically transmitting the recycled content score to the customer.

[0260] In one embodiment, the amount of recycled content in the recycled plastic feedstock or recycled PIA will be based on an allocation or credit obtained by the manufacturer of the recycled PIA composition, or the amount available in the quota catalog of the recycled PIA manufacturer. A portion or all of the allocation or credit obtained or owned by the manufacturer of the recycled PIA may be designated and allocated to the recycled plastic feedstock or recycled PIA based on mass balance. The allocated value of the recycled content of the recycled plastic feedstock or recycled PIA shall not exceed the total amount of all allocations and / or credits available to the manufacturer of the recycled PIA or other entity authorized to allocate recycled content values to the recycled PIA.

[0261] There is also provided a method of introducing or establishing recycled content in a compound, composition, polymer, and / or article without having to use a reactant compound or composition having recycled content.

[0262] In this method,

[0263] a. A syngas manufacturer prepares a syngas stream derived from recycled plastics, and

[0264] b. A polymer and / or article manufacturer:

[0265] i. Obtains a quota derived from gasified recycled plastics or from the syngas stream derived from the recycled plastics, from the syngas manufacturer or a third party transferring the quota,

[0266] ii. Prepares a polymer and / or article from any reactant compound or composition, and

[0267] iii. Associates at least a portion of the quota with at least a portion of the polymer and / or article, regardless of whether the reactant compound or composition used to prepare the polymer and / or article contains recycled content.

[0268] In this method, the polymer and / or article manufacturer does not need to purchase recycled reactant compounds or compositions from a specific source or supplier, and it is not required that the polymer and / or article manufacturer use or purchase reactant compounds or compositions having recycled content to successfully establish recycled content in the polymer and / or article composition. The polymer or article manufacturer may use reactant compounds or compositions from any source and apply at least a portion of the allocation or credit to at least a portion of the reactant compound or composition feedstock or at least a portion of the polymer and / or article product. The association by the polymer and / or article manufacturer may take any form, whether through a catalog, internal accounting methods, or a statement or claim made to a third party or the public.

[0269] There is also provided the use of a reactant compound or composition, which includes converting recycled pre-ground plastics in any synthesis process such as gasification to prepare syngas and / or recycled PIA.

[0270] There is also provided a use of recycled pre-ground plastics, which includes converting reactant compounds or compositions during synthesis to prepare polymers and / or articles, and applying at least a portion of the quota of the polymers and / or articles to the reactant compounds or compositions, wherein the quota is derived from gasifying a feedstock containing solid fossil fuels and recycled pre-ground plastics, or from a quota catalog, wherein at least one item entering the catalog is deposited from a feedstock gasifying containing solid fossil fuels and recycled pre-ground plastics.

[0271] In one embodiment, there is provided a polymer and / or article composition obtained by any of the above methods.

[0272] Reactant compounds or compositions, for example, reactant compounds or compositions can be stored in storage containers and transported to a recycled PIA manufacturing facility by truck, pipeline, or ship, or as further described below, a reactant compound or composition manufacturing facility can be integrated with a recycled PIA facility. Reactant compounds or compositions can be transported or transferred to an operator or facility for preparing polymers and / or articles.

[0273] In one embodiment, the method for preparing recycled PIA can be an integrated method. One such example is a method for preparing recycled PIA by the following steps:

[0274] a. Gasifying a feedstock containing solid fossil fuels and recycled pre-ground plastics to prepare a recycled-derived synthesis gas stream; and

[0275] b. Reacting the recycled-derived synthesis gas or non-recycled content synthesis gas prepared in a gasifier in a reaction scheme to prepare reactant compounds or compositions;

[0276] c. Reacting any reactant compounds or compositions during synthesis to prepare polymers and / or articles;

[0277] d. Depositing a quota into a quota catalog, the quota being derived from gasifying a feedstock containing solid fossil fuels and recycled pre-ground plastics; and

[0278] e. Applying any quota from the catalog to the polymers and / or articles to obtain a recycled content polymer and / or article composition.

[0279] In one embodiment, two or more facilities can be integrated and recycled PIA can be prepared. The facilities for preparing recycled PIA, reactant compounds or compositions, or synthesis gas can be independent facilities or facilities integrated with each other. For example, a system for producing and consuming reactant compounds or compositions can be established as follows:

[0280] a. Provide a reactant compound or composition manufacturing facility configured to produce a reactant compound or composition;

[0281] b. Provide a polymer and / or article manufacturing facility having a reactor configured to receive a reactant compound or composition from the reactant compound or composition manufacturing facility and prepare a polymer and / or article; and

[0282] c. Provide a supply system in fluid communication between the two facilities, the supply system being capable of supplying the reactant compound or composition from the reactant compound or composition manufacturing facility to the polymer and / or article manufacturing facility,

[0283] wherein the reactant compound or composition manufacturing facility generates a quota by gasifying a feedstock containing solid fossil fuel and recycled pre-ground plastic, and:

[0284] (i) The quota is applied to the reactant compound or composition, or to the polymer and / or article reactant, or

[0285] (ii) Deposited in a quota catalog, and any quota is withdrawn from the catalog and applied to the reactant compound or composition or polymer and / or article.

[0286] The reactant compound or composition manufacturing facility can apply the recycled content to the polymer and / or article by receiving any reactant compound or composition from the reactant compound or composition manufacturing facility, and by deducting the quota from its catalog and optionally applying them in an amount using the above method to the polymer and / or article prepared with the reactant compound or composition, thereby preparing recycled PIA. The quota withdrawn from the catalog and applied can be a quota obtained from any source of recycled content and does not have to be a quota associated with gasifying recycled pre-ground plastic.

[0287] In one embodiment, a system for producing recycled PIA is also provided:

[0288] a. Provide a gasification manufacturing facility configured to produce an output composition containing a recycled-derived synthesis gas stream;

[0289] b. Provide a reactant compound or composition manufacturing facility configured to receive the recycled-derived synthesis gas stream from the gasification manufacturing facility and prepare one or more downstream products of the synthesis gas through a reaction scheme to produce an output composition containing a reactant compound or composition;

[0290] c. Provide a polymer and / or article manufacturing facility having a reactor configured to receive the reactant compound or composition and prepare an output composition containing recycled-content recycled PIA; and

[0291] d. A supply system that provides fluid communication between at least two of these facilities and is capable of supplying the output composition of one manufacturing facility to another or more of the said manufacturing facilities.

[0292] The polymer and / or article manufacturing facility can prepare recycled PIA. In this system, the gasification manufacturing facility can make its output in fluid communication with the reactant compound or composition manufacturing facility, and in turn, the reactant compound or composition manufacturing facility can make its output in fluid communication with the polymer and / or article manufacturing facility. Alternatively, the manufacturing facilities of a) and b) can be in separate fluid communication, or only b) and c) in fluid communication. In the latter case, the polymer and / or article manufacturing facility can directly prepare recycled PIA by continuously converting the pre-ground plastic-containing syngas produced in the gasification manufacturing facility into recycled PIA, or indirectly prepare recycled PIA by receiving any reactant compound or composition from the reactant compound or composition manufacturing facility and applying recycled content to the recycled PIA by deducting a quota from its catalog and applying the amount thereof that can optionally use the above method. The quota obtained and stored in the catalog can be obtained by any of the above methods.

[0293] The fluid communication can be gaseous, liquid, or both. The fluid communication does not need to be continuous and can be interrupted by storage tanks, valves, or other purification or treatment facilities, as long as the fluid can be transported from the manufacturing facility to the subsequent facility through an interconnected pipeline network and without using trucks, trains, ships, or airplanes. Additionally, the facilities can share the same site, or in other words, one site can contain two or more facilities. Furthermore, the facilities can also share a storage tank site or storage tanks for auxiliary chemicals, or can also share utilities, steam, or other heat sources, etc., but are still considered separate facilities because their unit operations are separate. Facilities are typically defined by battery limits.

[0294] In one embodiment, the integrated process includes at least two facilities that are co-located within 5 miles, or 3 miles, or 2 miles, or 1 mile (as a straight-line measurement) of each other. In one embodiment, at least two facilities are owned by the same entity family.

[0295] In one embodiment, an integrated recycled PIA production and consumption system is also provided. The system includes:

[0296] a. A gasification manufacturing facility configured to produce an output composition comprising a recycled-derived syngas stream obtained by gasifying solid fossil fuels and recycled pre-ground plastics;

[0297] b. Provide a reactant compound or composition manufacturing facility configured to receive a recycled-derived synthesis gas stream from a gasification manufacturing facility and prepare one or more downstream products of the synthesis gas via a reaction scheme to manufacture an output composition comprising the reactant compound or composition;

[0298] c. Provide a polymer and / or article manufacturing facility having a reactor configured to receive the reactant compound or composition and prepare an output composition comprising the polymer and / or article; and

[0299] d. A piping system interconnecting at least two of the facilities, optionally interconnecting with intermediate processing equipment or storage facilities, the piping system capable of withdrawing an output composition from one facility and receiving the output at any one or more of the other facilities.

[0300] The system does not necessarily require fluid communication between the two facilities, although fluid communication is desirable. For example, the recycled-derived synthesis gas can be transported to the reactant compound or composition facility via an interconnected pipeline network, which can be interrupted by other processing equipment such as equipment for treatment, purification, pumping, compression, or equipment suitable for merging streams or storage facilities, all of which facilities can include optional metering, valves, or interlock equipment. The equipment can be fixed to the ground or fixed to a structure fixed to the ground. The interconnected pipelines do not need to be connected to the reactant compound or composition reactor or cracker, but rather to the transfer and receiving points at the respective facilities. The interconnected pipeline system does not need to connect all three facilities to each other, but rather the interconnected pipeline system can be between facilities a)-b), or b)-c), or between a)-b)-c).

[0301] In one embodiment, the total amount of carbon in the pre-ground plastic added to the solid fossil fuel is at least 70 wt.%, or at least 75 wt.%, or at least 80 wt.%.

[0302] The total amount of hydrogen in the pre-ground plastic is desirably at least 5 wt.%, or at least 8 wt.%, or at least 10 wt.%.

[0303] In another embodiment, the ratio of total hydrogen to total carbon in the plastic feed is higher than that in the solid fossil fuel. In one embodiment or in combination with any of the embodiments mentioned, in the pre-ground plastic used in the feedstock, the ratio of total hydrogen to total carbon is at least 0.075, or at least 0.08, or at least 0.085, or at least 0.09, or at least 0.095, or at least 0.1, or at least 0.11, or at least 0.12, or at least 0.13.

[0304] In another embodiment, the average fixed carbon content of the pre-ground plastic used in the feed stream is less than 75 wt.%, or not greater than 70 wt.%, or not greater than 65 wt.%, or not greater than 60 wt.%, or not greater than 55 wt.%, or not greater than 45 wt.%, or not greater than 40 wt.%, or not greater than 35 wt.%, or not greater than 30 wt.%, or not greater than 25 wt.%, or not greater than 20 wt.%, or not greater than 15 wt.%, or not greater than 10 wt.%, or not greater than 8 wt.%, or not greater than 6 wt.%, or not greater than 5 wt.%, or not greater than 4 wt.%, or not greater than 3 wt.%, or not greater than 2 wt.%, or not greater than 1 wt.%, based on the weight of the pre-ground plastic. The fixed carbon content is the combustible solid (excluding ash) remaining after the coal is heated and the volatiles are removed. It can be determined by subtracting the percentages of moisture, volatile matter, and ash from the sample. If there is a large mismatch in the fixed carbon content of the solids, the change in the syngas composition may exceed the desired limit. For example, in an entrainment flow high-temperature gasifier, solids with a very low fixed carbon content can be gasified more easily than coal, progressing from producing carbon monoxide to producing more carbon dioxide within the residence time experienced by the coal, while co-feeding of solids with a much higher fixed carbon content than coal will take longer to gasify and produce more unreacted solids. The extent of the syngas composition change that can be tolerated will depend on the use of the syngas, and in the case of preparing chemicals, it is desirable to minimize factors that may cause a wider syngas composition change. In the method of the present invention, since the plastic concentration in the solids is kept low, the change in the syngas composition due to the use of plastic can be ignored.

[0305] In another embodiment, the average fixed carbon content of the pre-ground plastic used in the feed stream is at least 3%, or at least 5%, or at least 7%, or at least 9%, or at least 10%, or at least 13%, or at least 15%, or at least 17%, or at least 20%, or at least 23%, or at least 25%, or at least 27%, or at least 30%, or at least 32%, or at least 35%, or at least 38%, or at least 40%, or at least 43%, or at least 45%, or at least 47%, or at least 50%, or at least 55%, or at least 60%, or at least 70%, or at least 80%, or at least 90%, or at least 95% less than that of coal, or all solid fossil fuels employed in the feed stream, or optionally any solid other than plastic.

[0306] The pre-ground plastic may have a low or only trace average sulfur content. The average sulfur content of the pre-ground plastic is at most 5 wt.%, or at most 4 wt.%, or at most 3.5 wt.%, or at most 3 wt.%, or at most 2.5 wt.%, or at most 2 wt.%, or at most 1.5 wt.%, or at most 1 wt.%, or at most 0.5 wt.%, or at most 0.25 wt.%, or at most 0.1 wt.%, or at most 0.05 wt.%, or at most 0.01 wt.%, or at most 0.005 wt.%, based on the weight of the pre-ground plastic.

[0307] The pre-ground plastic may have a widely varying ash content, depending on the type of plastic in the plastic stream and the purity of the selected plastic in the plastic stream. Based on the weight of the pre-ground plastic, the average ash content of the pre-ground plastic can be at least 1 wt.%, or at least 2 wt.%, or at least 3 wt.%, or at least 4 wt.%, or at least 10 wt.%, or at least 15 wt.%, or at least 20 wt.%, or at least 25 wt.%, or at least 30 wt.%, or at least 35 wt.%, or at least 40 wt.%, or at least 45 wt.%. Based on the weight of the pre-ground plastic, the average ash content of the pre-ground plastic can be more than 60 wt.%, or not greater than 55 wt.%, or not greater than 40 wt.%, or not greater than 30 wt.%, or not greater than 20 wt.%, or not greater than 15 wt.%, or not greater than 10 wt.%, desirably not greater than 8 wt.%, or not greater than 7 wt.%, or not greater than 6 wt.%, or not greater than 5.5 wt.%, or not greater than 5 wt.%, or not greater than 4.5 wt.%, or not greater than 4 wt.%, or not greater than 3 wt.%, or not greater than 2.5 wt.%.

[0308] In another embodiment, the average oxygen content in the plastic can be zero or at least 0.1 wt.%, or at least 0.5 wt.%, or at least 1 wt.%, or at least 2 wt.%, or at least 4 wt.%, or at least 6 wt.%, or at least 8 wt.%, or at least 10 wt.%, or at least 13 wt.%, or at least 15 wt.%, or at least 18 wt.%, or at least 20 wt.%. Desirably, in order to improve the HHV, a low oxygen content is maintained, such as not greater than 20 wt.%, or not greater than 15 wt.%, or not greater than 10 wt.%, or not greater than 8 wt.%, or not greater than 5 wt.%, or not greater than 4 wt.%, or not greater than 2 wt.%, or not greater than 1 wt.%, based on the weight of the pre-ground plastic.

[0309] In the pre - ground plastic, the content of minerals, metals, and elements other than carbon, hydrogen, oxygen, nitrogen, and sulfur can be at least 0.01 wt.%, or at least 0.1 wt.%, or at least 0.5 wt.%, or at least 1 wt.%, or at least 1.5 wt.%, or at least 1.8 wt.%, or at least 2 wt.%, or at least 2.3 wt.%, or at least 2.5 wt.%, or at least 2.8 wt.%, or at least 3 wt.%, based on the weight of the pre - ground plastic. There is no particular limitation on the upper limit, and it is generally not more than 8 wt.%, or not more than 7 wt.%, or not more than 6 wt.%, or not more than 5 wt.%, or not more than 4.5 wt.%, or not more than 4 wt.%, or not more than 3.8 wt.%.

[0310] The plastic added to the gasifier has been processed through at least one granulation step to reduce the size of the plastic from its original form or from the form of shredded / chipped plastic having an average size with the longest dimension of 1 / 4 inch or greater. Desirably, the plastic has been processed by a first - pass granulation or shredding from its original form before reaching the gasification facility. Then the coarsely granulated plastic is further finely granulated and optionally further shredded or ground to the final desired particle size. The gasification facility can receive the pre - granulated plastic at its final particle size, or can receive the coarsely ground plastic, and the operator / owner of the gasification equipment can perform the granulation steps necessary to obtain the desired particle size present in the feed stream.

[0311] The plastic is ground before being added to other fossil fuels, which means grinding them before combining them with solid fossil fuels and optionally but desirably screening them to the final particle size (“pre - ground plastic”). As described below, plastic of the original size, or coarsely ground plastic (e.g., having an average maximum size of 1 / 4 inch or greater, or even 0.5 inch or greater) cannot be processed by an entrained - flow coal gasifier. In addition, the elasticity of the plastic makes it unsuitable for co - granulation with harder and more brittle carbon - containing fuel sources such as coal or petroleum coke.

[0312] Pre-grind the plastic to a suitable particle size, optionally screen it, and then combine it with one or more fossil fuel components of the feed stream at any location before introducing the feed stream into the gasification zone within the gasifier. As described above, plastics are not easily pre-ground simultaneously in the same equipment used for grinding coal, especially in a slurry, because many plastics are soft, elastic, and not easily fragmented. However, the coal grinding equipment will provide an excellent energy source for mixing the pre-ground plastic with the fossil fuel while reducing the size of the coal particles. Thus, one desired location for combining the pre-ground plastic of a target size for feeding into the gasifier is into the equipment used for grinding other carbonaceous fossil fuel sources (such as coal, petroleum coke). In a slurry-fed gasifier, this location is particularly attractive because it is desired to use a feed with the highest possible stable solid concentration, and at higher solid concentrations, the viscosity of the slurry is also high. The torque and shear forces used in the fossil fuel grinding equipment are high, and combined with the shear-thinning behavior of the coal slurry, good mixing of the pre-ground plastic with the ground fossil fuel can be achieved in the fossil fuel grinding equipment.

[0313] Other locations for combining the pre-ground plastic with the fossil fuel source can be on the fossil fuel loaded on the main fossil fuel conveyor belt feeding the grinder, or on the main fossil fuel conveyor belt feeding the grinder before the fossil fuel is loaded onto the conveyor belt, or into a storage tank containing the fossil fuel slurry ground to its final size, especially if the storage tank is agitated.

[0314] There are several sites that provide a safe, economical, and effective way to introduce pre-ground solid plastics, including recycled plastics, into a slurry-fed coal gasifier. In additional embodiments of the present invention, Figure 5 Four locations where the recycled plastic content can be introduced are shown. All of these points are in the low-pressure section of the process (below the pressure in the gasifier or within the gasification zone), thus reducing the cost of the modification.

[0315] At Figure 5In the embodiment of the present invention shown, the recycled plastic content can be introduced at position 100, i.e., the main coal feed conveyor belt. As the main coal feed conveyor belt moves together with the coal feed already loaded on the conveyor belt, the plastic is metered onto the main coal feed conveyor belt. A weigh belt feeder or other similar device is used to add the plastic to the conveyor belt to measure the mass of the material and measure the speed of the conveyor belt to determine the addition rate. Coal is similarly added to the same conveyor belt and will be under the plastic. Then, a combined solid mixture of coal and plastic in the appropriate proportion is conveyed to a buffer hopper and other storage and conveying equipment until it is finally fed into a coal mill. In the coal mill, the coal, plastic, water, and viscosity modifier are thoroughly mixed, and the size of the coal is reduced to the target grinding size distribution, and the mixture becomes a viscous slurry. Since the plastic is a softer material, it undergoes very little or no reduction in diameter, but benefits from the extreme mixing in the mill due to its incorporation into the slurry production process. The plastic has been pre-ground to the target size (e.g., less than 2 mm) and does not require any further reduction in diameter.

[0316] In another embodiment of the present invention, as Figure 5 shown by position number 110, the recycled plastic content can be introduced. This is the same process as described in position 100 above, except that the plastic is added to the main coal conveyor belt first before adding the coal. In this way, the coal is on top. Since the plastic will be pre-ground and may inherently be less dense than the coal, this material may be more likely to be blown off the conveyor belt by strong winds. Since the coarser and denser coal covers the recycled material, this dust and material loss will be greatly reduced.

[0317] In another embodiment of the present invention, the recycled plastic content can be added at position number 120, the coal mill. Existing equipment, coal, water, and viscosity modifier have already been added to the coal mill to reduce the particle size of the coal and produce a viscous slurry with a high solid content. The plastic can be independently conveyed to the inlet point of the coal mill and added directly to the coal mill in the appropriate proportion. Then, in the process, the coal mill will grind the coal, produce the slurry, and mix it thoroughly with the plastic. This avoids the influence of wind and weather on the coal and recycled material mixture.

[0318] In another embodiment of the present invention, the recycled plastic content can be introduced at location 130, i.e., the slurry storage tank. Since the plastic is pre-ground to an appropriate particle size for introduction into the gasifier, it can be added directly to the slurry storage tank after the grinding / slurry operation. Alternatively, it can be added to the tank through a separate screen or the screen used by the slurry to ensure that no large particles enter the tank. This is the last low-pressure addition point before the slurry is pumped to the gasifier under pressure. This will minimize the amount of material mixed together during processing. Stirring in the slurry tank will mix in the plastic to ensure its uniform distribution.

[0319] For a variety of purposes, the fossil fuel (coal or petroleum coke) and plastic are ground or milled. The plastic must be ground to small sizes, and the fossil fuel source must also be ground to small sizes to (i) allow for faster reactions once inside the gasifier due to mass transfer limitations, (ii) produce a stable, fluid slurry at a high concentration of solids relative to water, and (iii) pass through processing equipment with tight clearances, such as high-pressure pumps, valves, and feed injectors. Generally, this means that the solids in the feedstock, including the plastic, are ground to a particle size of 2 mm or less. As used throughout the text, the particle size means that at least 90 wt.% of the particles have a maximum size within the stated size, or alternatively, 90 wt.% pass through a screen designated for that particle size. Either condition satisfies the particle size designation. Larger-sized plastics have the possibility of being blown through the gasification zone without being fully gasified, especially when the gasification conditions are established to gasify solid fossil fuels with a particle size of 2 mm or less.

[0320] The plastic is desirably ground to such a particle size that, after optional sieving, the particle size is acceptable for gasification within the design parameters of the gasifier. Desirably, the particle size of the plastic used in the feedstock, or the particle size of the plastic fed to or mixed with the solid fuel, is 2 mm or less, or passes through 10 mesh, or 1.7 mm or less (those particles passing through 12 mesh), or 1.4 mm or less (those particles passing through 14 mesh), or 1.2 mm or less (those particles passing through 16 mesh), or 1 mm or less (those particles passing through 18 mesh), or 0.85 mm or less (those particles passing through 20 mesh), or 0.7 mm or less (those particles passing through 25 mesh), or 0.6 mm or less (those particles passing through 30 mesh), or 0.5 mm or less (those particles passing through 35 mesh), or 0.4 mm or less (those particles passing through 40 mesh), or 0.35 mm or less (those particles passing through 45 mesh), or 0.3 mm or less (those particles passing through 50 mesh), or 0.25 mm or less (those particles passing through 60 mesh), or 0.15 mm or less (those particles passing through 100 mesh), or 0.1 mm or less (those particles passing through 140 mesh), or 0.07 mm or less (those particles passing through 200 mesh), or 0.044 mm or less (those particles passing through 325 mesh), or 0.037 mm or less (those particles passing through 400 mesh). In another embodiment, the size of the ground plastic particles is at least 0.037 mm (or 90% retained on 400 mesh). A sample of the pre-ground plastic will be considered to be within the stated particle size limits if 90 vol.% of the sample is within the specified limits.

[0321] In one embodiment or in combination with any of the embodiments mentioned, 90% of the particle size of the pre-ground plastic used in the feedstock composition is 1 mm or less, or 0.5 mm or less, or 0.25 mm or less, or 0.1 mm or less (or those particles passing through 140 mesh), or 0.07 mm or less (those particles passing through 200 mesh), or 0.044 mm or less (those particles passing through 325 mesh), or 0.037 mm or less (those particles passing through 400 mesh).

[0322] In another embodiment, the particle sizes of the rubber and the fossil fuel can be sufficiently matched to maintain the stability of the slurry and avoid coal / plastic separation at high solid concentrations before entering the gasification zone in the gasifier. A feed stream that phase separates, whether between solids / liquids or plastics / fossil fuels, can clog pipelines, create local areas of gasified plastic, create inconsistent fossil fuel / plastic ratios, and can affect the consistency of the syngas composition. Variables considered in determining the optimal particle size of the ground plastic include the bulk density of the ground coal, the concentration of all solids in the slurry if a slurry is used, the effectiveness of any additives such as surfactants / stabilizers / viscosity modifiers used, and the velocity and turbulence of the feed stream entering the gasifier and passing through the injector nozzle.

[0323] In one embodiment or in combination with any of the embodiments mentioned, the bulk density of the uncompacted (loose) ground plastic after final grinding is within 150%, or within 110%, or within 100%, or within 75%, or within 60%, or within 55%, or within 50%, or within 45%, or within 40%, or within 35% of the loose bulk density of the ground fossil fuel after its final grinding. For example, if the pelletized coal has a bulk density of 40 lbs / ft 3 and the pelletized plastic has a loose bulk density of 33 lbs / ft 3 then the bulk density of the plastic will be within 21% of the ground coal. For measurement purposes, the bulk density of the pre-ground plastic and fossil fuel after final grinding is determined dry (without adding water), even if they are ultimately used as a slurry.

[0324] In an alternative embodiment or in addition to any other embodiment described herein, the maximum particle size of the ground plastic is selected to be similar to (lower than or higher than) the maximum particle size of the ground coal. The maximum particle size of the ground plastic is desirably within 50%, or within 45%, or within 40%, or within 35%, or within 30%, or within 25%, or within 20%, or within 15%, or within 10%, or within 5% of (referring to lower than or higher than) the maximum particle size of the ground coal. The maximum particle size is not determined as the largest size of the particle distribution, but is determined by screening through sieve openings. The maximum particle size is determined as the first sieve opening that allows at least 90 volume % of the ground particle sample to pass through. For example, if less than 90 volume % of the sample passes through 300 mesh, then through 100 mesh, 50 mesh, 30 mesh, 16 mesh, but successfully passes through 14 mesh, then the maximum particle size of the sample is considered to correspond to the first sieve opening size that allows at least 90 volume % to pass through, and in this case, 14 mesh corresponds to a maximum particle size of 1.4 mm.

[0325] The amount of ground plastic present in the feed stream can be at most 25 wt.%, or at most 20 wt.%, or at most 15 wt.%, or at most 12 wt.%, or at most 10 wt.%, or at most 7 wt.%, or at most 5 wt.%, or less than 5 wt.%, or from 0.1 wt.% to 25 wt.%, or from 0.1 wt.% to 20 wt.%, or from 0.1 wt.% to 15 wt.%, or from 0.1 wt.% to 12 wt.%, or from 0.1 wt.% to 10 wt.%, or from 0.1 wt.% to 7 wt.%, desirably from 0.1 wt.% to at most or less than 5 wt.%, based on the weight of all solids. Since plastics on average have a much lower fixed carbon content than solid fossil fuels, they will produce a greater amount of carbon dioxide than solid fossil fuels in the gasification zone at the same residence time and based on the same weight. Desirably, the concentration of pre-ground plastic is low to obtain the advantage of minimizing the increase in the carbon dioxide content that exceeds the increase in the carbon dioxide content produced by solid fossil fuels alone. Desirably, the concentration of pre-ground plastic is less than 5 wt.%, or not more than 4.5 wt.%, or not more than 4 wt.%, or not more than 3.5 wt.%, or not more than 3 wt.%, or not more than 2.5 wt.%, or not more than 2 wt.%, and in each case at least 0.1 wt.%, or at least 0.5 wt.%, or at least 1 wt.%, each based on the weight of the solids in the feed stream. Examples of the content of ground plastic present in the feed stream include from 0.25 wt.% to less than 5 wt.%, or from 0.25 wt.% to 4 wt.%, or from 0.25 wt.% to 3 wt.%, or from 0.25 wt.% to 2.5 wt.%, or from 0.5 wt.% to 5 wt.%, or from 0.5 wt.% to 4 wt.%, or from 0.5 wt.% to 3 wt.%, or from 0.5 wt.% to 2.5 wt.%, or from 1 wt.% to 5 wt.%, or from 1 wt.% to 4 wt.%, or from 1 wt.% to 3 wt.%, or from 1 wt.% to 2.5 wt.%, each based on the weight of the solids in the feed stream. These ranges are particularly useful when using a mixed plastic stream.

[0326] The pre-ground plastic is desirably segregated as a ground plastic feed for mixing with one or more components of the feed stream at a final destination. In one embodiment or in combination with any of the embodiments mentioned, at least 80 wt.%, or at least 85 wt.%, or at least 90 wt.%, or at least 95 wt.%, or at least 96 wt.%, or at least 97 wt.%, or at least 98 wt.%, or at least 99 wt.%, or at least 99.5 wt.%, or 100 wt.% of all solid feedstocks other than solid fossil fuels in the feed stream to the gasifier is pre-ground plastic.

[0327] The solids in the feed stream are desirably free of sewage sludge, waste paper or biomass. In one embodiment or in combination with any of the embodiments mentioned, the feed stream contains any one of sewage sludge, waste paper, biomass, or a combination of two or more thereof, in an amount not greater than 10 wt.%, or not greater than 6 wt.%, or not greater than 5 wt.%, or not greater than 4 wt.%, or not greater than 3 wt.%, or not greater than 2 wt.%, or not greater than 1 wt.%, or not greater than 0.5 wt.%, or not greater than 0.25 wt.%, or not greater than 0.1 wt.%, each based on the weight of the solids in the feed stream.

[0328] Even after final grinding, the pre-ground plastic will contain a certain level of other materials such as metals, fillers and other materials. Based on the weight of the pre-ground plastic particles, the amount of such materials other than rubber fed into the feed stream in the pre-ground plastic is desirably less than 8 wt.%, or not greater than 6 wt.%, or not greater than 5 wt.%, or not greater than 4 wt.%, or not greater than 3.5 wt.%, or not greater than 2 wt.%, or not greater than 1.5 wt.%, or not greater than 1 wt.%, or not greater than 0.75 wt.%, or not greater than 0.5 wt.%.

[0329] The amount of solid fossil fuel such as coal in the feedstock or fed to the gasifier can be at least 10 wt.%, or at least 80 wt.%, or at least 85 wt.%, or at least 90 wt.%, or at least 93 wt.%, or at least 95 wt.%, or at least 97 wt.%, or at least 98 wt.%, or at least 98.5 wt.%, or at least 99 wt.% and less than 100 wt.%, or less than 99.5 wt.%, based on the weight of the solids in the feedstock.

[0330] Coal contains a certain amount of ash, and the ash also contains elements other than carbon, oxygen and hydrogen. Based on the weight of all dry solids in the feed stream, or alternatively based on the weight in the feed stream, the amount of elements other than carbon, hydrogen, oxygen and sulfur in the feed stream is desirably not greater than 9 wt.%, or not greater than 8.5 wt.%, or not greater than 8 wt.%, or not greater than 7.5 wt.%, or not greater than 7 wt.%, or not greater than 6.5 wt.%, or not greater than 6 wt.%, or not greater than 5.5 wt.%, or not greater than 5 wt.%, or not greater than 4.5 wt.%.

[0331] The calorific value of plastics is desirably similar to or better than that of coal. For example, the calorific value of plastics is at least 13,000, or at least 13,500, or at least 14,000 BTU / lb, or in the range of 13,000 to 15,000 BTU / lb (30 MJ / Kg - 35 MJ / Kg), while bituminous coal may have a calorific value in the range of 12,500 to 13,300 BTU / lb (29 - 31 MJ / Kg). In addition, any ash or non-organic materials will be melted and vitrified into the ash or slag matrix produced by the inorganic matter in coal. Therefore, plastics can be regarded as a direct substitute for coal in the feeding process.

[0332] The concentration of solids (such as fossil fuels and plastics) in the feed stream should not exceed the stability limit of the slurry, or be no greater than the ability to pump or supply the feedstock to the gasifier at the target solid concentration. Desirably, the solid content of the slurry should be at least 50 wt.%, or at least 55 wt.%, or at least 60 wt.%, or at least 62 wt.%, or at least 65 wt.%, or at least 68 wt.%, or at least 69 wt.%, or at least 70 wt.%, or at least 75 wt.%, with the remainder being the liquid phase which may contain water and liquid additives. There is no particular limit on the upper limit as it depends on the gasifier design. However, considering the practical pumpability limitations of solid fossil fuel feeding and maintaining a uniform distribution of solids in the slurry, the solid content for slagging gasifiers with solid fossil slurry feeding should desirably not exceed 75 wt.% or 73 wt.%, with the remainder being the liquid phase which may include water and liquid additives (as mentioned above, gas is not included in the calculation of weight percentages).

[0333] The feed stream is desirably stable for 5 minutes, or even 10 minutes, or even 15 minutes, or even 20 minutes, or even half an hour, or even 1 hour, or even two hours. The feed slurry is considered stable if the initial viscosity of the feed slurry is 100,000 cP or lower. The initial viscosity can be obtained by the following method. At ambient conditions (e.g., 25 °C and about 1 atm), 500 - 600 g of a well - mixed sample is allowed to stand in a 600 mL glass beaker. After the slurry is well - mixed (e.g., forming a uniform distribution of solids), a Brookfield R / S rheometer equipped with a V80 - 40 vane and operating at a shear rate of 1.83 / s is immersed into the slurry to the bottom of the beaker. After a specified period of time, a viscosity reading is obtained at the start of rotation, which is the initial viscosity reading. If the initial reading at the start of viscosity measurement at the specified period is not greater than 100,000 cP, the slurry is considered stable. Alternatively, the same procedure can be used with a Brookfield viscometer equipped with an LV - 2 spindle and rotating at a rate of 0.5 rpm. Since different viscosities will be obtained using different equipment, the type of equipment used should be reported. However, regardless of the differences, under either method, the slurry is considered stable only if its viscosity is not greater than 100,000 cP within the reported time.

[0334] Adjust the amount of solids and their particle size in the feed stream to maximize the solid content while maintaining a stable and pumpable slurry. A pumpable slurry is a slurry that has a viscosity of less than 30,000 cP, or not greater than 25,000 cP, or not greater than 23,000 cP, and desirably not greater than 20,000 cP, or not greater than 18,000 cP, or not greater than 15,000 cP, or not greater than 13,000 cP in each case at ambient conditions (e.g., 25 °C and 1 atm). At higher viscosities, the slurry becomes too thick to be practically pumped. Viscosity measurements to determine the pumpability of the slurry are made by mixing a slurry sample until a uniform distribution of particles is obtained, then immediately immersing a Brookfield viscometer equipped with an LV - 2 spindle and rotating at a rate of 0.5 rpm into the well - mixed slurry and reading the value without delay. Alternatively, a Brookfield R / S rheometer equipped with a V80 - 40 vane spindle and operating at a shear rate of 1.83 / s can be used. Report the measurement method because the values measured at their different shear rates between the two rheometers will produce different values. However, the above cP values apply to either the rheometer equipment and procedure.

[0335] Conventional plastic granulators can be used to obtain the desired particle size. These can include systems that use high-capacity shredders to cut the plastic into pieces, followed by granulation, and if needed, a fine / powder granulator can be used in the final step. For the final step, the fine / powder granulator can be connected to a conveying system to convey the granulated plastic to a storage container from which the granulated plastic can be fed to any location for preparing the feed stream, or the granulated pellets can be continuously fed from the fine granulator to the desired location for preparing the feed stream. Feeding the granulated plastic particles from the storage container can be in batch mode or continuous mode.

[0336] Carbonaceous materials, such as fossil fuels and plastics, are advantageously loose and are not compacted by mechanical or chemical means after final granulation to prepare pre-ground plastics (except for natural compaction that may occur due to storage under their own weight), or desirably at any time before preparing the pre-ground plastics and after their post-industrial manufacture or post-consumer use. For example, coal lumps are granulated in the presence of water and are not compacted thereafter, and plastics are finely ground / crushed without a compaction operation before they are added to water.

[0337] For the reasons stated above, coal must be ground before being fed to the gasifier to obtain an acceptable particle size. These same considerations apply to plastic particles, although as noted above, since coal grinding equipment is not suitable for grinding plastics, the plastics must be pre-ground before being combined with the feed composition or before being added to the coal grinding equipment.

[0338] Coal is typically ground to a size of 2 mm or less and can be ground to any size as described above for the granulated plastic particles. The small size of the coal and plastic particles is important for ensuring uniform suspension in the liquid carrier without settling, allowing sufficient movement relative to the gaseous reactants, ensuring substantially complete gasification, and providing a pumpable slurry with a high solids content with minimal grinding.

[0339] The quality of the coal used is not restricted. Anthracite, bituminous coal, sub-bituminous coal, lignite, and peat can be sources of the coal feedstock. To improve the thermal efficiency of the gasifier, the carbon content of the coal used is desirably more than 35 wt.%, or at least 42 wt.%, based on the weight of the coal. Thus, bituminous coal or anthracite is ideal due to its higher energy content.

[0340] Sulfur is also typically present in solid fossil fuels. Desirably, the sulfur content is less than 5 wt.%, not more than 4 wt.%, or not more than 3 wt.%, or not more than 2.5 wt.%, and can also include measures of sulfur, such as at least 0.25 wt.%, or at least 0.5 wt.%, or at least 0.75 wt.%.

[0341] It is also desirable to use coal with a low inherent moisture content to improve the thermal efficiency of the gasifier. It is desirable to use coal with a moisture content of less than 25 wt.%, or less than 20 wt.%, or less than 15 wt.%, or not more than 10 wt.%, or not more than 8 wt.% without applying externally applied heat.

[0342] Desirably, the calorific value of the coal feedstock is at least 11,000 BTU / lb, or at least 11,500 BTU / lb, or at least 12,500 BTU / lb, or at least 13,000 BTU / lb, or at least 13,500 BTU / lb, or at least 14,000 BTU / lb, or at least 14,250 BTU / lb, or at least 14,500 BTU / lb.

[0343] Although the feed stream may contain a small amount of liquid hydrocarbon oil leached from plastics or coal, the feed stream desirably contains less than 5 wt.%, or not more than 3 wt.%, or not more than 1 wt.%, or not more than 0.1 wt.% of liquid (under ambient conditions) non-oxidized hydrocarbon oil, which is introduced into the feed stream as is. Desirably, the feed stream contains less than 2 wt.%, or not more than 1 wt.%, or no added liquid fractions from refined crude oil or reformed any such fractions. Desirably, the amount of liquid in the feed stream is different from the solid content. The liquid content or water content present in the feed stream desirably is not more than 50 wt.%, or not more than 35 wt.%, or not more than 32 wt.%, or not more than 31 wt.%, or not more than 30 wt.%, based on the weight of the feed stream. Desirably, in each case, the content of liquid or water in the feed stream desirably is at least 10 wt.%, or at least 15 wt.%, or at least 20 wt.%, or at least 25 wt.%, or at least 27 wt.%, or at least 30 wt.%, based on the weight of the feed stream. Desirably, based on the weight of all liquids fed to the gasifier, the liquid present in the feed stream contains at least 95 wt.%, or at least 96 wt.%, or at least 97 wt.%, or at least 98 wt.%, or at least 99 wt.% of water. In another embodiment, except for chemically synthesized chemical additives containing oxygen or sulfur or nitrogen atoms, the liquid content of the feed stream is at least 96 wt.%, or at least 97 wt.%, or at least 98 wt.%, or at least 99 wt.% of water, based on the weight of all liquids fed to the gasifier.

[0344] In one embodiment, the water present in the feed stream is not wastewater, or in other words, the water fed to the solids to prepare the feed stream is not wastewater. Desirably, the water used is not industrially discharged from any process of synthetic chemicals, or it is not municipal wastewater. The water is desirably fresh water or drinking water.

[0345] The feedstock stream includes at least ground coal and ground plastic. Desirably, the feedstock stream also contains water. The amount of water in the feedstock stream can be 0 wt.% to 50 wt.%, or 10 wt.% to 40 wt.%, or 20 wt.% to 35 wt.%. The feedstock stream is desirably an aqueous slurry.

[0346] In addition to coal, water, and plastic, other additives can be added to and included in the feedstock stream, such as viscosity modifiers and pH regulators. The total amount of additives can be 0.01 wt.% - 5 wt.%, or 0.05 wt.% - 3 wt.%, or 0.5 wt.% - 2.5 wt.% based on the weight of the feedstock stream. The amount of any individual additive can also be within these ranges.

[0347] Viscosity modifiers (which include surfactants) can improve the solids concentration in the slurry. Examples of viscosity modifiers include:

[0348] (i) Alkyl-substituted amine-based surfactants, such as alkyl-substituted aminobutyric acids, alkyl-substituted polyethoxyamides, alkyl-substituted polyethoxy quaternary ammonium salts, etc.; and

[0349] (ii) Sulfates, such as organic sulfonates, including ammonium sulfonate, calcium sulfonate, and sodium sulfonate, especially those with lignin and sulfonated alkylated lignite;

[0350] (iii) Phosphates;

[0351] (iv) Polyoxyalkylene anionic or nonionic surfactants.

[0352] More specific examples of alkyl-substituted aminobutyric acid surfactants include N-coco-β-aminobutyric acid, N-tallow-β-aminobutyric acid, N-lauryl-β-aminobutyric acid, and N-oleyl-β-aminobutyric acid. N-coco-β-aminobutyric acid.

[0353] More specific examples of alkyl-substituted polyethoxyamide surfactants include polyoxyethylene oleamide, polyoxyethylene tallowamide, polyoxyethylene laurylamide, and polyoxyethylene cocoamide, where there are 5 - 50 polyoxyethylene moieties.

[0354] More specific examples of alkyl-substituted polyethoxy quaternary ammonium salt surfactants include methyl bis(2-hydroxyethyl) cocoammonium chloride, methyl polyoxyethylene cocoammonium chloride, methyl bis(2-hydroxyethyl) oleylammonium chloride, methyl polyoxyethylene oleylammonium chloride, methyl bis(2-hydroxyethyl) stearylammonium chloride, and methyl polyoxyethylene stearylammonium chloride.

[0355] More specific examples of sulfonates include sulfonated formaldehyde condensates, naphthalene sulfonate formaldehyde condensates, benzenesulfonate-phenol-formaldehyde condensates, and lignosulfonates.

[0356] More specific examples of phosphates include trisodium phosphate, potassium phosphate, ammonium phosphate, sodium tripolyphosphate or potassium tripolyphosphate.

[0357] Examples of polyoxyalkylene anionic or nonionic surfactants have one or more repeating units derived from ethylene oxide or propylene oxide, or 1 - 200 oxyalkylene units.

[0358] Desirably, the surfactant is an anionic surfactant such as an organic sulfonic acid. Examples are calcium, sodium and ammonium salts of organic sulfonic acids such as 2,6 - dihydroxynaphthalene sulfonic acid, lignite sulfonic acid and ammonium lignosulfonate.

[0359] Examples of pH regulators include aqueous solutions of alkali metal and alkaline earth metal hydroxides such as sodium hydroxide, and ammonium compounds such as 20 - 50 wt.% aqueous ammonium hydroxide. The aqueous ammonium hydroxide solution can be added directly to the feedstock composition before entering the gasifier, for example in a coal grinding device or any downstream vessel containing the slurry.

[0360] The total oxygen to carbon atomic ratio entering the gasification zone can be a value in the range of 0.70 to less than 2, or 0.9 to 1.9, or 0.9 to 1.8, or 0.9 to 1.5, or 0.9 to 1.4, or 0.9 to 1.2, or 1 to 1.9, or 1 to 1.8, or 1 to 1.5, or 1 to 1.2, or 1.05 to 1.9, or 1.05 to 1.8, or 1.05 to 1.5, or 1.05 to 1.2. The free oxygen to carbon atomic ratio entering the gasification zone can also be within these same values. The total oxygen and free oxygen to carbon weight ratios (in pounds) entering the gasification zone can also each be within these stated values.

[0361] The total carbon content in the feedstock stream is at least 40 wt.%, or at least 45 wt.%, or at least 50 wt.%, or at least 55 wt.%, or at least 60 wt.%, or at least 65 wt.%, and desirably at least 70 wt.%, or at least 75 wt.%, or at least 80 wt.%, or at least 85 wt.%, or at least 90 wt.%, each based on the total solids content.

[0362] The feedstock stream is desirably injected with an oxidant into the combustion chamber of the refractory lining of the syngas - generating gasifier. The feedstock stream (desirably a slurry) and the oxidant are desirably injected into the gasification zone under significant pressure, typically about 500 psig or higher, or 600 psig or higher, or 800 psig or higher, or 1000 psig or higher. The velocity or flow rate of the feedstock and oxidant streams injected from the injector nozzle into the combustion chamber will exceed the rate of flame propagation to avoid flashback.

[0363] In one embodiment or in combination with any of the embodiments of the present invention, advantageously only one feed stream is added to the gasifier or the gasification zone, or in other words, all carbon fuel sources are fed to the gasifier in only one stream. In another embodiment, only one feed stream is required or used to produce a syngas or product stream, which is a feedstock for synthetic compounds.

[0364] In another embodiment, chemicals are made from a first syngas that is derived from a first gasifier that is fed a first feed stream containing coal, and the first syngas stream is not combined with a second syngas that is derived from any other gasifier that is fed a second feed stream, where the coal content difference between the first and second feed streams is greater than 20%, or greater than 10%, or greater than 5%. For example, a first syngas stream generated from a first feed stream containing 90 wt.% coal will not be combined with a syngas stream generated from a different gasifier fed a feed stream containing 70 wt.% coal or no coal, but may be combined with a syngas stream containing 72 wt.% coal or more coal.

[0365] Before entering the gasifier, the feed stream may be subjected to a variety of other optional processes. For example, a coal-rubber slurry may flow through a thickener in which excess water is removed from the slurry to obtain the final desired solids concentration of the slurry entering the gasifier vessel. Additionally, the feed stream may be preheated before entering the gasifier. In this embodiment, the feed stream is heated to a temperature below the boiling point of water at the operating pressure present in the reaction zone. When a preheater is used, the preheater reduces the heat load on the gasifier and increases the utilization efficiency of both the fuel and the oxygen. In this embodiment, all of the water required to produce syngas in the reaction zone is supplied in the liquid phase. When petroleum coke is used as the fuel for the gas generator, a portion of the water, such as 1 - about 90 wt.% of the water based on the weight of the water, may be evaporated in the slurry feed preheater or as evaporated water combined with the oxygen stream.

[0366] The oxidant is desirably an oxidizing gas, which may include air, and desirably is an oxygen-rich gas in an amount greater than that found in air. The reaction of oxygen with solid fossil fuel is exothermic. Desirably, based on the total moles in the oxidant gas stream injected into the reaction (combustion) zone of the gasifier, the oxidant gas contains at least 25 mole% oxygen, or at least 35 mole%, or at least 40 mole%, or at least 50 mole%, or at least 70 mole%, or at least 85 mole%, or at least 90 mole%, or at least 95 mole%, or at least 97 mole%, or at least 98 mole% oxygen, or at least 99 mole%, or at least 99.5 mole%. In another embodiment, the total concentration of oxygen in all the gases supplied to the gasification zone is also the above amount. Considering the amount of the feedstock stream, the amount of the feed, the process conditions, and the gasifier design, the specific amount of oxygen supplied to the reaction zone is desirably sufficient to obtain carbon monoxide and hydrogen from the gasification reaction that is close to or the maximum yield relative to the components in the feedstock stream.

[0367] In one embodiment or in combination with any of the embodiments mentioned, steam is not supplied to the gasification zone. The amount of water in the slurry feed system is generally greater than that required to satisfy the co-reactant and the heat sink to regulate the gasification temperature. Adding a stream in a slurry feed gasifier will generally undesirably absorb heat from the reaction zone and reduce its efficiency.

[0368] Other reducible oxygen-containing gases can be supplied to the reaction zone, such as carbon dioxide, nitrogen, or simply air. In one embodiment or in combination with any of the embodiments mentioned, no gas stream rich in carbon dioxide or nitrogen (e.g., greater than the molar amount present in air, or greater than 2 mole%, or greater than 5 mole%, or greater than 10 mole%, or greater than 40 mole%) is charged into the gasifier. Many of these gases are used as carrier gases to push the dry feed into the gasification zone. Due to the pressure in the gasification zone, these carrier gases are compressed to provide the power for introduction into the gasification zone. Avoiding the consumption of energy and equipment for compressing the carrier gas to the feedstock stream is the slurry feed. Thus, in another embodiment, the feedstock stream flowing to the gasifier that contains at least pre-ground material and ground solid fossil fuel, or this feedstock stream introduced into the injector or the feed pipe, or this feedstock stream introduced into the gasification zone, or a combination of all of the above, does not contain gas compressed in a gas compression device. Alternatively or additionally, except for the above-mentioned oxygen-rich stream, no gas compressed in a gas compression device is fed into the gasification zone or even into the gasifier. It should be noted that the high-pressure feed pump for processing the slurry feed introduced into the gasification zone is not considered a gas compression device.

[0369] Desirably, no gas stream containing more than 0.03 mole%, or more than 0.02 mole%, or more than 0.01 mole% carbon dioxide is added to the gasifier or the gasification zone. In another embodiment, no gas stream containing more than 77 mole%, or more than 70 mole%, or more than 50 mole%, or more than 30 mole%, or more than 10 mole%, or more than 5 mole%, or more than 3 mole% nitrogen is added to the gasifier or the gasification zone. In another embodiment, steam is not added to the gasification zone or the gasifier. In yet another embodiment, a gaseous hydrogen stream (e.g., a gaseous hydrogen stream containing more than 0.1 mole% hydrogen, or more than 0.5 mole%, or more than 1 mole%, or more than 5 mole% hydrogen) is not added to the gasifier or the gasification zone. In another embodiment, a methane gas stream (e.g., a methane gas stream containing more than 0.1 mole% methane, or more than 0.5 mole%, or more than 1 mole%, or more than 5 mole% methane) is not added to the gasifier or the gasification zone. In another embodiment, the only gas stream introduced into the gasification zone is the oxygen-rich gas stream as described above.

[0370] The gasification method desirably employed is the partial oxidation gasification reaction. To increase the production of hydrogen and carbon monoxide, the oxidation process involves the partial rather than complete oxidation of the fossil fuel and the plastic, and thus desirably operates in an oxygen-lean environment relative to the amount required for 100% carbon and hydrogen bond oxidation. The total oxygen requirement of the gasifier desirably exceeds the amount required to convert the carbon content of the solid fuel and the plastic into carbon monoxide by at least 5%, or at least 10%, or at least 15%, or at least 20% in theory. Generally, satisfactory operation can be obtained with a total oxygen supply of 10% to 80% above the theoretical requirement. Examples of the appropriate amount of oxygen per pound of carbon are 0.4 to about 3.0 pounds of free oxygen per pound of carbon, or 0.6 to 2.5, or 0.9 to 2.5, or 1 to 2.5, or 1.1 to 2.5, or 1.2 to 2.5 pounds of free oxygen.

[0371] The mixing of the feed stream and the oxidizer is desirably completed entirely within the reaction zone by introducing separate streams of the feed and the oxidizer such that they impinge on each other within the reaction zone. Desirably, the oxidizer stream is introduced into the reaction zone of the gasifier at a high velocity to both exceed the flame propagation rate and improve the mixing with the feed stream. The oxidizer is desirably injected into the gasification zone at a rate in the range of 25 to 500 feet per second, or 50 to 400 feet per second, or 100 to 400 feet per second. These values will be the velocity of the gaseous oxidizing stream at the injector-gasification zone interface, or the injector tip velocity.

[0372] One method for increasing the velocity of the oxidizer feed to the gasification zone is by reducing the diameter of the oxidizer annulus near the injector or the injector tip. Near the top of the injector, the annular channel is at Figure 3 and4 The hollow cone shown converges inwardly. Thus, the oxidizing gas is accelerated and discharged from the injector as a high-speed conical flow having an apex angle in the desirable range of about 30° to 45°. The flow from the injector converges at a point located about 0 - 6 inches outside the injector surface. The high-speed oxidizing gas flow impinges on the relatively low-speed feedstock flow, atomizes it, and forms a fine mist that contains tiny particles of water and particulate solid carbonaceous fuel highly dispersed in the oxidizing gas. The particles of the solid carbonaceous material impinge on each other and further break up.

[0373] The velocity of the feedstock slurry is determined by the desired production rate of syngas generation. A suitable example of the velocity of the feedstock introduced into the gasification zone prior to contact with the oxidizer is 5 - 50 feet per second.

[0374] The feedstock stream and the oxidizer can optionally be preheated to a temperature above about 200°C, or at least 300°C, or at least 400°C. Advantageously, the gasification process employed does not require preheating the feedstock stream to effectively gasify the fuel, and the preheating treatment step would result in a reduction in the energy efficiency of the process. Desirably, the feedstock stream and the optional oxidizer are not preheated before they are introduced into the gasifier. The preheating treatment step would be to bring the feedstock stream or the oxidizer into contact with a device that sufficiently raises the temperature of the feedstock stream such that the temperature of the feedstock stream or the oxidizer stream is immediately above 200°C, or above 190°C, or above 170°C, or above 150°C, or above 130°C, or above 110°C, or above 100°C, or above 98°C, or above 90°C, or above 80°C, or above 70°C, or above 60°C before being introduced into the injector on the gasifier. For example, although coal can be dried with hot air above 200°C, if the feedstock stream is below 200°C when introduced into the injector, this step would not be considered preheating of the feedstock stream.

[0375] In another embodiment, no thermal energy (except for incidental heat from processing equipment such as mills, grinders, or pumps) is applied to the feedstock stream containing plastic and solid fossil fuel, or to the oxidizer stream, at any point (except for the temperature rise experienced in the injector) before the feedstock stream containing plastic and solid fossil fuel is introduced into the injector or the gasifier or the gasification zone, such that the thermal energy would raise the temperature of the stream by more than 180°C, or more than 170°C, or more than 160°C, or more than 150°C, or more than 140°C, or more than 130°C, or more than 120°C, or more than 110°C, or more than 100°C, or more than 90°C, or more than 80°C, or more than 70°C, or more than 60°C, or more than 50°C, or more than 40°C, or more than 30°C.

[0376] The method of the present invention employs a gasification process, which is different from pyrolysis (a thermal process that degrades a fuel source in the absence of air or oxygen) or plasma processes, as gasification does not utilize a plasma arc.

[0377] Desirably, the type of gasification technology employed is a partial oxidation entrained flow gasifier that produces syngas. This technology is different from fixed bed (or moving bed) gasifiers and fluidized bed gasifiers. In a fixed bed (or moving bed gasifier), the feed stream and the oxidant gas move in a countercurrent flow manner, and the oxidant gas commonly used is air. The feed stream falls into the gasification chamber, accumulates, and forms a feed bed. Air (or alternatively oxygen) continuously flows upward from the bottom of the gasifier through the bed of feed material, while fresh feed continuously falls from the top due to gravity to renew the bed during bed combustion. The combustion temperature is typically lower than the melting temperature of the ash and does not slag. Regardless of whether the fixed bed operates in a countercurrent or, in some cases, a co-current manner, the fixed bed reaction process produces a large amount of tar, oil, and methane generated by the pyrolysis of the feed in the bed, thereby contaminating the produced syngas and the gasifier. The contaminated syngas requires a great deal of effort and cost to remove the tar-like residues, which will condense once the syngas cools, and thus, such a syngas stream is generally not used for chemical production but for direct heating applications. In a fluidized bed, the feed material in the gasification zone is fluidized by the action of an oxidant flowing through the bed at a high enough velocity to fluidize the particles in the bed. In a fluidized bed, the homogeneous reaction temperature and low reaction temperature in the gasification zone also promote the production of a large amount of unreacted feed material and low carbon conversion rate. The operating temperature in a fluidized bed is typically between 800 - 1000 °C. Additionally, in a fluidized bed, it is important to operate under slagging conditions to maintain the fluidization of the feed particles; otherwise, the feed particles will adhere to the slag and agglomerates. By using entrained flow gasification, these deficiencies present in fixed bed (or moving bed) and fluidized bed gasifiers commonly used for waste treatment are overcome.

[0378] In one embodiment or in combination with any of the embodiments mentioned, the feed stream is introduced at the top 1 / 8 portion of the gasifier, desirably at the top 1 / 12 of the gasifier height (excluding the injector height protruding from the top of the housing or the pipe protruding from the bottom of the housing) defined by the gasifier housing. The feed stream is desirably not introduced into the sidewall of the gasifier. In another embodiment, the feed stream is not a tangential feed injector.

[0379] In another embodiment, the oxidant is introduced into the top 1 / 8 portion of the gasifier, desirably at the top 1 / 12 of the gasifier height defined by the gasifier shell. The oxidant is desirably not introduced into the sidewalls or the bottom of the gasifier. In another embodiment, both the feed stream and the oxidant are introduced into the top 1 / 8 portion of the gasifier, desirably at the top 1 / 12 of the gasifier height defined by the gasifier shell. Desirably, the oxidant and the feed stream are fed in co-current to ensure good mixing. In this regard, co-current feeding means that the axes of the feed stream and the oxidant stream are substantially parallel (e.g., the deviation between them is not greater than 25°, or not greater than 20°, or not greater than 15°, or not greater than 10°, or not greater than 8°, or not greater than 6°, or not greater than 4°, or not greater than 2°, or not greater than 1°) and in the same direction.

[0380] The feed stream and the oxidant stream are desirably introduced into the gasification zone through one or more injector nozzles. Desirably, the gasifier is equipped with at least one injector nozzle through which the feed stream and the oxidant stream are introduced into the gasification zone.

[0381] Although the feed stream can be dry feed or slurry feed, the feed stream is desirably a slurry. The syngas produced during the gasification process is desirably at least partially used to prepare chemicals. Many synthetic methods for preparing chemicals are under high pressure, and in order to avoid energy input to pressurize the syngas stream, desirably, the gasifier also operates under high pressure, especially when the syngas stream is in direct or indirect gas communication with the vessel gas for synthesizing chemicals. The dry feed of the gasifier operating under high pressure is specially treated to ensure that the feed can be effectively blown and injected into the high-pressure gasification zone. Some techniques involve entraining a nitrogen gas stream under high pressure and high speed, which tends to dilute the syngas stream and reduce the concentration of desired components such as carbon monoxide and hydrogen. Other carrier gases or motive gases include carbon monoxide, but similar to nitrogen, these gases are compressed before being added to or compressed with the solid fossil fuel, increasing the energy requirements and capital costs of the feed lock hopper and / or compression equipment. To address these issues, many dry-feed gasifiers will operate at a lower pressure, which is sufficient for power generation only, but is not desirable for gasifiers that produce a syngas stream for manufacturing chemicals. For slurry feed, motive gas is not required and can be easily fed into a high-pressure gasifier that produces high-pressure syngas, which is desirable for manufacturing chemicals. In one embodiment or in combination with any of the embodiments mentioned, the feed stream is not processed through a lock hopper before entering the injector or the gasification zone. In another embodiment, the feed composition containing ground plastic and solid fossil fuel is not pressurized in a lock hopper.

[0382] Desirably, the gasifier is non-catalytic, meaning that the gasifier does not contain a catalyst bed, and desirably, the gasification process is non-catalytic, meaning that a catalyst is not introduced into the gasification zone as discrete unbound catalyst (as opposed to trapped metals in plastics or solid fossil fuels which may incidentally have catalytic activity). The gasification process in the reaction zone desirably proceeds without the addition of a catalyst and does not contain a catalyst bed. The gasification process is also desirably a slagging gasification process; i.e., operating under slagging conditions (well above the melting temperature of the ash) such that slag is formed in the gasification zone and flows downward along the refractory walls.

[0383] In another embodiment, the gasifier is not designed to contain a pyrolysis zone. Desirably, the gasifier is not designed to contain a combustion zone. Most preferably, the gasifier is designed to not contain, or effectively not contain, a combustion zone or a pyrolysis zone. A pyrolysis zone does not completely consume the fuel source, resulting in potentially large amounts of ash, char, and tarry products. A combustion zone, although not present in the tar, produces large amounts of CO2 and lesser amounts of the more desirable carbon monoxide and hydrogen. Desirably, the gasifier is a single-stage reactor, meaning that there is only one zone within the gasifier shell for converting carbon in the feedstock into gas.

[0384] The gasification zone is a void or empty space defined by walls where oxidation reactions occur and gases are allowed to form within that space. Desirably, the gasification zone does not have a molten pool of molten material or molten material accumulating at the bottom of the gasification zone to form a molten pool. The gasification zone is desirably not closed at the bottom but is in gas communication with other zones below the gasification zone. The slag does not accumulate at the bottom of the gasification zone upon melting but flows downward along the sides of the refractory and into a zone below the gasification zone, such as a quench zone, to solidify the slag.

[0385] The flow of hot raw syngas in the gasifier is desirably vertically downward, or a downflow reactor. Desirably, the syngas stream produced in the gasifier flows downward from the highest point of the injected feedstock stream, desirably from the point of all feedstock stream locations. In another embodiment, the location where the syngas stream is withdrawn from the gasifier is lower than at least one location where the feedstock stream is introduced, desirably lower than all locations where the feedstock stream is introduced.

[0386] The gasifier desirably contains a refractory lining in the gasification zone. While a steam generation membrane or jacket can be used between the gasifier wall and the surface facing the gasification zone, desirably, the gasifier does not contain a membrane wall, or a steam generation membrane, or a steam jacket in the gasification zone or between the inner surface facing the gasification zone and the gasifier shell wall, as this removes heat from the gasification zone. Desirably, the gasification zone is lined with refractory material, and optionally there is no air or steam or water jacket between the refractory lining of the gasification zone (or optionally in any reaction zone, such as combustion or pyrolysis) and the outer shell of the gasifier.

[0387] The gasification process is desirably a continuous process, meaning that the gasifier operates in a continuous mode. Incorporating pre-pelletized plastic into the feed stream can be intermittent or continuous, as long as a continuous feed of fossil fuel is fed into the gasifier, since the gasification process in the gasifier is in continuous mode. The continuous mode of gasifier operation means that the gasification process is continuous for at least 1 month, or at least 6 months, or at least 1 year. Desirably, incorporating pelletized plastic into the feed stream is continuous for at least 1 day, or at least 3 days, or at least 14 days, or at least 1 month, or at least 6 months, or at least 1 year. The process is considered continuous even though there may be downtime due to maintenance or repair.

[0388] The feedstock can be fed into the gasification zone through one or more injectors. In one embodiment or in combination with any of the embodiments mentioned, the gasifier contains only one injector. In another embodiment, the gasifier contains only one location for introducing the feedstock. Generally, the injector nozzle serving the gasification chamber is configured to cause the feedstock stream to concentrically surround the oxidant gas stream along the axial core of the nozzle. Optionally, the oxidant gas stream can also surround the feedstock stream ring as a larger, substantially concentric ring. Radially surrounding the outer wall of the outer oxidant gas passage can be an annular cooling water jacket that terminates in a substantially flat end radiator aligned in a plane substantially perpendicular to the nozzle discharge axis. Cooling water is directed from outside the combustion chamber to directly contact the back side of the radiator end face for conducting heat away.

[0389] The reaction between hydrocarbon and oxygen should occur entirely outside the injector to prevent local concentration of the combustible mixture at or near the surface of the injector element.

[0390] The gasification zone and optionally all reaction zones in the gasifier operate at temperatures in the range of at least 1000 °C, or at least 1100 °C, or at least 1200 °C, or at least 1250 °C, or at least 1300 °C, and at most about 2500 °C, or at most 2000 °C, or at most 1800 °C, or at most 1600 °C, each of which is far above the melting temperature of the ash, and desirably operates to form slag in the reaction zone. In one embodiment or in combination with any of the embodiments mentioned, the reaction temperature is desirably self-sustaining. Advantageously, a gasifier operating in a steady state mode is at a self-sustaining temperature and does not require the application of external energy to heat the gasification zone.

[0391] In one embodiment or in combination with any of the embodiments mentioned, the gasifier does not contain a zone within the gasifier housing for drying the feedstock such as coal, petroleum coke, or plastic before gasification. The temperature rise within the injector is not considered a zone for drying.

[0392] Desirably, the gasification zone is not under negative pressure during operation, but is under positive pressure during operation. The gasification zone is desirably not equipped with any suction device or other means to create negative pressure under steady state operation.

[0393] The gasifier operates at a pressure in the gasification zone (or combustion chamber) of at least 200 psig (1.38 MPa), or at least 300 psig (2.06 MPa), or at least 350 psig (2.41 MPa), and desirably at least 400 psig (2.76 MPa), or at least 420 psig (2.89 MPa), or at least 450 psig (3.10 MPa), or at least 475 psig (3.27 MPa), or at least 500 psig (3.44 MPa), or at least 550 psig (3.79 MPa), or at least 600 psig (4.13 MPa), or at least 650 psig (4.48 MPa), or at least 700 psig (4.82 MPa), or at least 750 psig (5.17 MPa), or at least 800 psig (5.51 MPa), or at least 900 psig (6.2 MPa), or at least 1000 psig (6.89 MPa), or at least 1100 psig (7.58 MPa), or at least 1200 psig (8.2 MPa). The specific operating pressure at the high end is adjusted according to various considerations, including operating efficiency, the operating pressure required in the chemical synthesis reactor, especially in a chemical synthesis reactor with integrated equipment, and the process chemistry. The suitable operating pressure in the gasification zone does not need to exceed 1300 psig (8.96 MPa) at the high end, or does not need to exceed 1250 psig (8.61 MPa), or does not need to exceed 1200 psig (8.27 MPa), or does not need to exceed 1150 psig (7.92 MPa), or does not need to exceed 1100 psig (7.58 MPa), or does not need to exceed 1050 psig (7.23 MPa), or does not need to exceed 1000 psig (6.89 MPa), or does not need to exceed 900 psig (6.2 MPa), or does not need to exceed 800 psig (5.51 MPa), or does not need to exceed 750 psig (5.17 MPa). Examples of suitable desired ranges include 400 to 1000, or 425 to 900, or 450 to 900, or 475 to 900, or 500 to 900, or 550 to 900, or 600 to 900, or 650 to 900, or 400 to 800, or 425 to 800, or 450 to 800, or 475 to 800, or 500 to 800, or 550 to 800, or 600 to 800, or 650 to 800, or 400 to 750, or 425 to 750, or 450 to 750, or 475 to 750, or 500 to 750, or 550 to 750, each in psig units.

[0394] Desirably, the average residence time of the gas in the gasifier reactor is desirably very short to increase production. Since the gasifier is desirably operated at high temperature and high pressure, the raw material can be substantially completely converted into gas within a very short time range. The average residence time of the gas in the gasifier can be as short as less than 30 seconds, or no greater than 25 seconds, or no greater than 20 seconds, or no greater than 15 seconds, or no greater than 10 seconds, or no greater than 7 seconds. Desirably, the average residence time of the gas in all regions designed to convert the raw material into gas is also very short, such as less than 25 seconds, or no greater than 15 seconds, or no greater than 10 seconds, or no greater than 7 seconds, or no greater than 4 seconds. Within these time ranges, at least 85 wt.%, or at least or greater than 90 wt.%, or at least 92 wt.%, or at least 94 wt.% of the solids in the raw material can be converted into gas (substances that remain gaseous if the gas stream is cooled to 25 °C and 1 atm) and liquids (substances that are liquid if the gas stream is cooled to 25 °C and 1 atm, such as water), or greater than 93 wt.%, or greater than 95 wt.%, or greater than 96 wt.%, or greater than 97 wt.%, or greater than 98 wt.%, or greater than 99 wt.%, or greater than 99.5 wt.%.

[0395] A portion of the ash and / or char in the gasifier can be entrained in the hot raw synthesis gas stream leaving the gasification reaction zone. The ash particles in the raw synthesis gas stream within the gasifier are particles that have not reached the melting temperature of the minerals in the solid fuel. The slag is essentially molten ash or molten ash that has solidified into glassy particles and remains within the gasifier. The slag melts until quenched and then forms beads of molten minerals. The char is a porous particle of fuel particles that have been devolatilized and partially burned (incomplete conversion). The particulate matter that accumulates at the bottom of the gasifier or in the quench zone is mainly slag (e.g., more than 80 wt.% slag), and the remainder is char and ash. Desirably, only trace amounts of tar or no tar are present in the gasifier, or in the quench zone, or in the gasification zone, or in the hot raw synthesis gas within the gasifier, or in the raw synthesis gas discharged from the gasifier (which can be determined by the amount of tar condensed from the synthesis gas stream when cooled to a temperature below 50 °C). Trace amounts are less than 0.1 wt.% of the solids present in the gasifier (or less than 0.05 wt.% or less than 0.01 wt.%), or less than 0.05 volume% of the raw synthesis gas stream discharged from the gasifier, or no greater than 0.01 volume%, or no greater than 0.005 volume%, or no greater than 0.001 volume%, or no greater than 0.0005 volume%, or no greater than 0.0001 volume%.

[0396] In another embodiment, relative to the same method, except that the same amount and type of solid fossil fuel used in the mixed raw material composition is substituted for plastic, the method does not increase the amount of tar to a significant extent.

[0397] In this process, the amount of tar produced with the mixed feedstock is higher by less than 10%, or less than 5%, or less than 3%, or less than 2%, or not higher at all, than the amount of tar produced with the same feedstock in which the plastic is replaced by the same solid fossil fuel under the same conditions.

[0398] To avoid fouling of the equipment downstream of the gasifier (scrubber, CO / H2 shift reactor, acid gas removal, chemical synthesis) and the intermediate pipelines, the synthesis gas stream should have a low tar content or no tar content. The synthesis gas stream exiting the gasifier desirably contains no tar or contains less than 4 wt.%, or less than 3 wt.%, or not more than 2 wt.%, or not more than 1 wt.%, or not more than 0.5 wt.%, or not more than 0.2 wt.%, or not more than 0.1 wt.%, or not more than 0.08 wt.%, or not more than 0.05 wt.%, or not more than 0.02 wt.%, or not more than 0.01 wt.%, or not more than 0.005 wt.% of tar, based on the weight of all condensable solids in the synthesis gas stream. For measurement purposes, condensable solids are those compounds and elements that condense at a temperature of 15 °C / 1 atm.

[0399] In another embodiment, the tar (if any) present in the synthesis gas stream exiting the gasifier is less than 10 g / m3, or not more than 9 g / m3, or not more than 8 g / m3, or not more than 7 g / m3, or not more than 6 g / m3, or not more than 5 g / m3, or not more than 4 g / m3, or not more than 3 g / m3, or not more than 2 g / m3, and desirably not more than 1 g / m3, or not more than 0.8 g / m3, or not more than 0.75 g / m3, or not more than 0.7 g / m3, or not more than 0.6 g / m3, or not more than 0.55 g / m3, or not more than 0.45 g / m3, or not more than 0.4 g / m3, or not more than 0.3 g / m3, or not more than 0.2 g / m3, or not more than 0.1 g / m3, or not more than 0.05 g / m3, or not more than 0.01 g / m3, or not more than 0.005 g / m3, or not more than 0.001 g / m3, or not more than 0.0005 g / m3, in each case at normal (15 °C / 1 atm). For measurement purposes, the tar is that which condenses at a temperature of 15 °C / 1 atm and includes primary, secondary, and tertiary tars, and is an aromatic organic compound and not ash, carbon, soot, or dust. Examples of tar products include naphthalene, cresol, xylenol, anthracene, phenanthrene, phenol, benzene, toluene, pyridine, catechol, biphenyl, benzofuran, benzaldehyde, acenaphthene, fluorene, naphthofuran, benzanthracene, pyrene, fluoranthene, benzo[a]pyrene, and other high molecular weight aromatic polynuclear compounds. The tar content can be determined by GC-MSD.

[0400] In another embodiment, the tar yield of the gasifier (the combination of tar in the syngas, tar at the bottom of the reactor, and tar in or on the ash, carbon, and slag) is not greater than 4 wt.%, or not greater than 3 wt.%, or not greater than 2.5 wt.%, or not greater than 2.0 wt.%, or not greater than 1.8 wt.%, or not greater than 1.5 wt.%, or not greater than 1.25 wt.%, or not greater than 1 wt.%, or not greater than 0.9 wt.%, or not greater than 0.8 wt.%, or not greater than 0.7 wt.%, or not greater than 0.5 wt.%, or not greater than 0.3 wt.%, or not greater than 0.2 wt.%, or not greater than 0.1 wt.%, or not greater than 0.05 wt.%, or not greater than 0.01 wt.%, or not greater than 0.005 wt.%, or not greater than 0.001 wt.%, or not greater than 0.0005 wt.%, or not greater than 0.0001 wt.%, based on the weight of the solids in the feedstock stream to the gasification zone.

[0401] Due to the gasification technology employed and the very small particle size of the plastic, the amount of carbon produced by gasifying the plastic-solid fossil fuel feedstock stream can be kept within acceptable limits. For example, the amount of carbon produced by converting the carbon source in the feedstock stream (or the unreacted carbon in the feedstock) is not greater than 15 wt.%, or not greater than 12 wt.%, or not greater than 10 wt.%, or not greater than 8 wt.%, or not greater than 5 wt.%, or not greater than 4.5 wt.%, or not greater than 4 wt.%, or not greater than 3.5 wt.%, or not greater than 3 wt.%, or not greater than 2.8 wt.%, or not greater than 2.5 wt.%, or not greater than 2.3 wt.%, or not greater than 4.5 wt.%, or not greater than 4.5 wt.%, or not greater than 4.5 wt.%.

[0402] In this method, the carbon can be recycled back into the feedstock stream. In another embodiment, the efficiency and characteristics of the present invention can be obtained without recycling the carbon back to the gasification zone.

[0403] The total amount of char (or unreacted carbon in the feedstock) and slag produced in or by the gasifier is desirably no greater than 20 wt.%, or no greater than 17 wt.%, or no greater than 15 wt.%, or no greater than 13 wt.%, or no greater than 10 wt.%, or no greater than 9 wt.%, or no greater than 8.9 wt.%, or no greater than 8.5 wt.%, or no greater than 8.3 wt.%, or no greater than 8 wt.%, or no greater than 7.9 wt.%, or no greater than 7.5 wt.%, or no greater than 7.3 wt.%, or no greater than 7 wt.%, or no greater than 6.9 wt.%, or no greater than 6.5 wt.%, or no greater than 6.3 wt.%, or no greater than 6 wt.%, or no greater than 5.9 wt.%, or no greater than 5.5 wt.%, in each case based on the weight of the solids in the feedstock stream. In another embodiment, the same values apply to the total amount of ash, slag, and char produced in or by the gasifier, based on the weight of the solids in the feedstock stream. In another embodiment, the same values apply to the total amount of ash, slag, char, and tar produced in or by the gasifier, based on the weight of the solids in the feedstock stream.

[0404] The raw synthesis gas stream flows from the gasification zone to the quench zone at the bottom of the gasifier, where the slag and the raw synthesis gas stream are cooled, typically to a temperature below 550 °C or below 500 °C or below 450 °C. The quench zone contains water in a liquid state. The hot synthesis gas from the gasification zone can be cooled by bringing the synthesis gas stream into direct contact with the liquid water. The synthesis gas stream can bubble through the liquid water pool or just contact the surface of the pool. Additionally, the hot synthesis gas stream can be cooled in a water jacket chamber having a height above the top surface of the pool to allow the hot synthesis gas to contact both the pool and be cooled in the water jacket chamber. The slag is solidified by the quench water, and most of the ash, slag, and char are transferred to the water in the quench tank. Then, the gas stream that has been partially cooled by the water in the quench zone can be discharged from the gasifier as the raw synthesis gas stream and passed through a water wash operation to remove any remaining entrained particulate matter.

[0405] The pressure in the quench zone is substantially the same as the pressure in the gasification zone above the water level in the gasifier, and a portion of the quench water and the solids at the bottom of the quench tank are removed through a lock hopper system. The quench water stream carrying fine particles exits the gasifier quench zone in response to a level controller and can be directed to a settler. The solids and water from the lock hopper can then flow into a water sump or a settler, where optionally the coarse particulate solids can be removed through a screen or a filter, resulting in a dispersion of fine particulate solids.

[0406] The raw gas stream discharged from the gasification vessel includes gases such as hydrogen, carbon monoxide, and carbon dioxide, and depending on the fuel source and reaction conditions, may include other gases such as methane, hydrogen sulfide, and nitrogen. The carbon dioxide in the raw syngas stream discharged from the gasification vessel desirably is present in an amount less than 20 mole%, or less than 18 mole%, or less than 15 mole%, or less than 13 mole%, or not more than 11 mole%, based on the total moles of the gases in the stream. Depending on the purity of the fuel and oxygen supplied to the process, some nitrogen and argon may be present in the raw syngas stream.

[0407] In one embodiment or in combination with any of the embodiments mentioned, the raw syngas stream (the stream discharged from the gasifier and before any further treatment by washing, shift conversion, or acid gas removal) may have the following composition, in mole% on a dry basis and based on the moles of all gases (elements or compounds in the gaseous state at 25 °C and 1 atm) in the raw syngas stream:

[0408] a. H 2 : 15 to 60, or 18 to 50, or 18 to 45, or 18 to 40, or 23 to 40, or 25 to 40, or 23 to 38, or 29 to 40, or 31 to 40

[0409] b. CO: 20 to 75, or 20 to 65, or 30 to 70, or 35 to 68, or 40 to 68, or 40 to 60, or 35 to 55, or 40 to 52

[0410] c. CO2: 1.0 to 30, or 2 to 25, or 2 to 21, or 10 to 25, or 10 to 20

[0411] d. H2O: 2.0 to 40.0, or 5 to 35, or 5 to 30, or 10 to 30

[0412] e. CH4: 0.0 to 30, or 0.01 to 15, or 0.01 to 10, or 0.01 to 8, or 0.01 to 7, or 0.01 to 5, or 0.01 to 3, or 0.1 to 1.5, or 0.1 to 1

[0413] f. H2S: 0.01 to 2.0, or 0.05 to 1.5, or 0.1 to 1, or 0.1 to 0.5

[0414] g. COS: 0.05 to 1.0, or 0.05 to 0.7, or 0.05 to 0.3

[0415] h. Total sulfur: 0.015 to 3.0, or 0.02 to 2, or 0.05 to 1.5, or 0.1 to 1

[0416] i. N2: 0.0 to 5, or 0.005 to 3, or 0.01 to 2, or 0.005 to 1, or 0.005 to 0.5, or 0.005 to 0.3

[0417] The gas components can be determined by FID-GC and TCD-GC or any other recognized method for analyzing the components of an air stream.

[0418] The hydrogen / carbon monoxide molar ratio is desirably at least 0.65, or at least 0.68, or at least 0.7, or at least 0.73, or at least 0.75, or at least 0.78, or at least 0.8, or at least 0.85, or at least 0.88, or at least 0.9, or at least 0.93, or at least 0.95, or at least 0.98, or at least 1.

[0419] On a dry basis, relative to the total amount of syngas discharged from the gasifier, the total amount of hydrogen and carbon monoxide is high, on the order of greater than 70 mole%, or at least 73 mole%, or at least 75 mole%, or at least 77 mole%, or at least 79 mole%, or at least 80 mole%, based on the discharged syngas.

[0420] In another embodiment, the dry syngas production rate, expressed as the volume of gas discharged from the gasifier per kilogram of solid fuel (such as plastics and coal) charged to all locations on the gasifier, is at least 1.7, or at least 1.75, or at least 1.8, or at least 1.85, or at least 1.87, or at least 1.9, or at least 1.95, or at least 1.97, or at least 2.0, in each case in Nm3 gas / kg of feed solids.

[0421] The single-pass carbon conversion rate is good and can be calculated according to the following formula:

[0422]

[0423] In this method, the single-pass carbon conversion efficiency can be at least 70%, or at least 73%, or at least 75%, or at least 77%, or at least 80%, or at least 82%, or at least 85%, or at least 88%, or at least 90%, or at least 93%.

[0424] In another embodiment, the amount of particulate solids in the raw synthesis gas stream is greater than 0 wt.% to at most 30 wt.%, or greater than 0 wt.% to at most 10 wt.%, or greater than 0 wt.% to at most 5 wt.%, or greater than 0 wt.% to at most 1 wt.%, or greater than 0 wt.% to at most 0.5 wt.%, or greater than 0 wt.% to at most 0.3 wt.%, or greater than 0 wt.% to at most 0.2 wt.%, or greater than 0 wt.% to at most 0.1 wt.%, or greater than 0 wt.% to at most 0.05 wt.%, each based on the weight of the solids in the feed stream. In this case, the amount of particulate solids is determined by cooling the synthesis gas stream to a temperature below 200 °C, such as occurs in a washing operation.

[0425] The percentage of cold gas efficiency of a method using a mixed plastic / solid fossil fuel can be calculated as:

[0426]

[0427] The cold gas efficiency is at least 60%, or at least 65%, or at least 66%, or at least 67%, or at least 68%, or at least 69%, or desirably at least 70%, or at least 71%, or at least 72%, or at least 73%, or at least 74%, or at least 75%, or at least 76%, or at least 77%, or at least 78%, or at least 79%.

[0428] In one embodiment or in combination with any of the embodiments mentioned, hydrogen and carbon monoxide from the raw synthesis gas stream discharged from the gasifier or from the washed or purified synthesis gas stream are not recovered or recycled back to the gasification zone in the gasifier. Desirably, carbon dioxide from the raw synthesis gas stream discharged from the gasifier or from the washed or purified synthesis gas stream is not recovered or recycled back to the gasification zone in the gasifier. Desirably, no portion of the synthesis gas stream discharged from the gasifier or from the washed or purified synthesis gas stream is recovered or recycled back to the gasification zone in the gasifier. In another embodiment, no portion of the syngas discharged from the gasifier is used to heat the gasifier. Desirably, no portion of the syngas produced in the gasifier is burned to dry the solid fossil fuel.

[0429] Under conditions sufficient to produce slag and ash, in an entrained flow reaction zone, the feed stream is desirably gasified with an oxidant such as oxygen. The slag and ash are separated from the syngas, quenched and solidified. In a partial oxidation reactor, a coal / plastic / water mixture is injected together with oxygen, and the coal / rubber will react with oxygen to produce various gases, including carbon monoxide and hydrogen (syngas). The slag and unreacted carbon / plastic accumulate in a pool in the quench zone at the bottom of the gasifier to cool and solidify these residues.

[0430] In one embodiment or in combination with any of the embodiments mentioned, the slag discharged from the gasifier is solid. The slag cools and solidifies in a quench zone within the gasifier housing of the gasifier and is discharged from the gasifier housing as a solid. This also applies to ash and carbon. These solids discharged from the gasifier accumulate in a lock hopper, and then the lock hopper can be emptied. The lock hopper is typically isolated from the gasifier and the quench zone within the gasifier.

[0431] The method can be implemented on an industrial scale and on a scale sufficient to produce synthesis gas as a raw material for the preparation of chemicals on an industrial scale. At least 300 tons per day, or at least 500 tons per day, or at least 750 tons per day, or at least 850 tons per day, or at least 1000 tons per day, or at least 1250 tons per day, and desirably at least 1500 tons per day, or at least 1750 tons per day, or even at least 2000 t / d of solids can be fed to the gasifier. The gasifier is desirably not designed to be movable but is fixed to the ground and is desirably stationary during operation.

[0432] The compositional variability of the synthesis gas produced by gasifying a feedstock containing solid fossil fuels and plastics is rather low over time. In one embodiment or in combination with any of the embodiments mentioned, during a period when the feedstock stream contains solid fossil fuels and pre-ground plastics, the compositional variability of the synthesis gas stream is low. The compositional variability of the synthesis gas stream can be determined by making at least 6 measurements of the concentration of relevant gaseous compounds in moles over equal time sub-periods throughout a time period when the solid content of the feedstock is consistent and contains plastics, and the entire time period does not exceed 12 days. The average concentration of the gaseous compounds is determined over the 6 measurements. The absolute value of the difference between the number farthest from the average and the average is determined and divided by the average x 100 to obtain the percentage of compositional variability.

[0433] The compositional variability of any of the following:

[0434] a. The amount of CO, or

[0435] b. The amount of H 2 or

[0436] c. The amount of CO2, or

[0437] d. The amount of CH4, or

[0438] e. The amount of H2S, or

[0439] f. The amount of COS, or

[0440] g. The amount of H2 + CO, or its stoichiometric molar ratio (e.g., H2:CO ratio), or

[0441] h. The amount of H2 + CO + CO2, or its stoichiometric molar ratio, or

[0442] i. The amount of H2 + CO + CH4, or their sequential molar ratios, or

[0443] j. The amount of H2 + CO + CO2 + CH4, or their sequential molar ratios, or

[0444] k. The amount of H2S + COS, or their sequential molar ratios, or

[0445] l. H2 + CO + CO 2 +CH 4 +H 2 S + COS,

[0446] Over a 12-day period or the shorter of the time the plastic is present in the feedstock composition, it can be no greater than 5%, or no greater than 4%, or no greater than 3%, or no greater than 2%, or no greater than 1%, or no greater than 0.5%, or no greater than 0.25%.

[0447] In another embodiment, the variability of the synthesis gas stream produced from a mixed feedstock containing plastic ("mixed case") is compared with the baseline variability of the synthesis gas stream produced from the same feedstock without plastic, where the amount of plastic is replaced by an equivalent amount of the same fossil fuel ("solid fossil fuel only case"), and processed under the same conditions to obtain % conversion variability, or in other words, the synthesis gas variability generated by switching between the two feedstock compositions. The variability of the mixed case can be less than or equivalent to or, if higher, similar to the variability of the solid fossil fuel only case. The period for determining the variability is set by the shorter of a 12-day period or the time the plastic is present in the feedstock composition, and this period is the same as the period used for measurement in the solid fossil fuel only case. The measurements for the solid fossil fuel only case are made within 1 month before or after the expiration of feeding the plastic-containing feedstock to the gasifier. The variability of the synthesis gas composition produced by each stream is measured according to the above procedure. The synthesis gas mixed case variability is less than or equal to or no greater than 15%, or no greater than 10%, or no greater than 5%, or no greater than 4%, or no greater than 3%, or no greater than 2%, or no greater than 1%, or no greater than 0.5%, or no greater than 0.25% of the synthesis gas solid fossil fuel only case. This can be calculated as:

[0448]

[0449] where %SW is the percentage of synthesis gas switching variability of one or more measured components in the synthesis gas composition; and

[0450] V m is the synthesis gas composition variability using the mixed stream containing plastic and fossil fuel; and

[0451] V ff is the syngas compositional variability using only fossil fuel streams, where the solid concentration is the same in both cases, the fossil fuel is the same in both cases, and the feedstock is gasified under the same conditions, rather than temperature fluctuations, which may vary spontaneously due to the presence of plastics in the feedstock, and the variability is relative to any one or more of the syngas compounds determined above. In cases where %SV is negative, the syngas mixing variability is less than the syngas only solid fossil fuel case.

[0452] In another embodiment, the ratio of carbon monoxide / hydrogen produced from a stream of plastic and solid fossil fuel (mixed stream) is similar to the carbon monoxide / hydrogen ratio produced from the same stream with the plastic content replaced by the same solid fossil fuel (only ff stream). The carbon monoxide / hydrogen ratio between the mixed stream and the only ff stream can differ from each other within 10%, or within 8%, or within 6%, or within 5%, or within 4%, or within 3%, or within 2%, or within 1.5%, or within 1%, or within 0.5%. The similarity percentage can be calculated by taking the absolute value of the difference in the CO / H 2 ratio and dividing that number by the CO / H of the only ff stream 2 ratio x 100.

[0453] In another embodiment, the amount of CO2 produced from a stream of plastic and solid fossil fuel (mixed stream) is similar to the amount of carbon dioxide produced from only the ff stream. The method of the present invention can be carried out such that the amount of CO 2 produced from a stream of plastic and solid fossil fuel (mixed stream) is no greater than 25%, or no greater than 20%, or no greater than 15%, or no greater than 13%, or no greater than 10%, or no greater than 8%, or no greater than 7%, or no greater than 6%, or no greater than 5%, or no greater than 4%, or no greater than 3%, or no greater than 2%, or no greater than 1%, or no greater than 0.75%, or no greater than 0.5%, or no greater than 0.25%, or no greater than 0.15%, or no greater than 0.1% of the amount of carbon dioxide produced from only the ff stream (e.g., coal). The similarity percentage can be calculated by subtracting the amount of CO 2 produced in the syngas stream using the mixed stream from the amount of CO 2 produced in the syngas stream using only the ff stream and dividing that number by the CO2 x 100 produced in the syngas stream using only the ff stream.

[0454] In another embodiment, a continuous method is provided for feeding a continuous feed composition containing solid fossil fuel to a gasifier and intermittently feeding a feed composition containing plastic and solid fossil fuel while maintaining negative, zero, or minimal syngas composition conversion variability over time ranges including feeds with and without plastic, using the syngas produced from the feed without plastic as a reference. For example, the switching frequency between a feed without plastic (only FF) and the same feed with a portion of the solid replaced by plastic (mixed) can be at least 52x / yr, or at least 48x / yr, or at least 36x / yr, or at least 24x / yr, or at least 12x / yr, or at least 6x / yr, or at least 4x / yr, or at least 2x / yr, or at least 1x / 2yr, and up to 3x / 2yr without triggering more than the above percentage of syngas switching variability. A switch is counted as the number of times the mixed feed is used within a time period.

[0455] To illustrate an embodiment of the overall method, reference is made to Figure 1 . Coal is fed through line 1 into a coal grinding zone 2 where it is mixed with water from stream 3 and ground to the desired particle size. Suitable coal grinding processes include shear processes. Examples of suitable equipment include ball mills, rod mills, hammer mills, Raymond mills, or ultrasonic mills; ideally a rod mill. The rod mill is desirably of the wet grinding type to prepare a slurry. The rod mill contains many rods within a cylinder where the rods rotate about a horizontal axis or close to a horizontal axis. The coal is ground when it is caught between the rods and the cylinder wall by the rolling / rotating action of the rods. The rod mill can be of the overflow type, end peripheral discharge, and central peripheral discharge, desirably the overflow type.

[0456] The grinder can also be equipped with a classifier to remove particles larger than the target maximum particle size. An example of a classifier is a vibrating screen or a weir screw classifier.

[0457] The coal grinding zone (which includes at least the grinding equipment, the feed mechanism of the grinder, and any classifier) is a convenient location for incorporating pre-ground plastic particles through line 4 into the coal. The required amounts of coal and plastic can be combined on a weighing belt or fed separately through their dedicated weighing belts to the grinding equipment. The water slurry of the ground coal and plastic is discharged through line 5 and pumped into a storage / feed tank 6 which is desirably agitated to maintain a uniform slurry suspension. Alternatively, or in addition to the location of the grinder 2, the pre-ground plastic can be added through line 7 to the feed / storage tank 6, especially when the tank is agitated.

[0458] The feed stream is discharged from the tank 6 directly or indirectly into the gasifier 9, enters the injector 10 through the pipeline 8, where the coal / rubber / water slurry is co-injected with the oxygen-rich gas from the pipeline 11 into the gasification reaction zone 12, where combustion occurs. The injector 10 can optionally be cooled by a water pipeline 13 with a jacket added to the injector and discharged through the pipeline 14. After startup and in the steady state, the reaction in the reaction zone 12 proceeds spontaneously at an autogenous temperature within the above range, such as 1200 - 1600 °C, and at a pressure within the above range, such as 10 - 100 atmospheres. The gaseous reaction products of the partial oxidation reaction include carbon monoxide, hydrogen, and smaller amounts of carbon dioxide and hydrogen sulfide. Molten ash, unreacted coal or rubber, and slag may also be present in the reaction zone 12.

[0459] The gasifier 9 is shown in Figure 2 more detail, as also shown in U.S. Patent 3,544,291, the entire disclosure of which is incorporated herein by reference. The gasifier includes a cylindrical pressure vessel 50 having a refractory lining 75 that defines a cylindrical, compact, unfilled reaction zone 54. A mixture of coal, plastic, water, and oxygen is axially injected through an inlet passage 76 into the upper end of the reaction zone 54 through an injector. The reaction products are axially discharged from the lower end of the reaction zone 54 through an outlet passage 77 into a slag quench chamber 71. The quench chamber 71 and the reaction zone 54 are within the outer shell 50 of the gasifier and are continuously in gas and fluid communication with each other during combustion and reaction in the reaction zone 54. A water pool 78 is maintained at the lower part of the quench chamber 71, and a water jacket 79 is provided at the upper part of the quench chamber 71 to protect the pressure vessel shell from being overheated by the hot gases from the gasification zone 54. Unreacted solid fuel and slag, as well as ash from the solid fuel, are discharged into the quench chamber 71 together with the product gas stream, where the larger particles of the solid and any molten ash or slag fall into the water pool. The partially cooled gas is discharged from the quench chamber 71 through line 58, which optionally also has a refractory lining 75.

[0460] Returning to Figure 1, the hot reaction product gas from the reaction zone 12, together with the slag formed on the refractory surface facing the reaction zone 12, is discharged into the quench chamber 15, where they are rapidly cooled and solidified in zone 12 at a temperature below the reaction temperature to form solid slag, ash, and unreacted coal, which are separated from the hot raw synthesis gas to form a raw synthesis gas stream that is discharged from the gasifier vessel. This method achieves the separation of ash, slag, and unreacted products from the reaction product gas and has advantages over fixed-bed or moving-bed waste gasifiers because, within the gasifier vessel, a first step of purifying the gaseous reaction products from the reaction zone 12 has occurred before the raw synthesis gas stream is discharged from the gasification vessel. At the same time, the slag and the gasified unreacted fossil fuel components solidify in the quench water in the quench zone 15, and a portion of the quench water vaporizes to produce steam, which can be used for subsequent operations, such as the water-gas shift reaction of the raw synthesis gas stream for washing, where hydrogen is produced by the reaction of carbon monoxide with steam in the presence of a suitable catalyst such as an iron oxide-chromium oxide catalyst.

[0461] The temperature of the raw synthesis gas stream leaving the gasification vessel through line 16 can be in the range of 150 °C to 700 °C or 175 °C to 500 °C. Desirably, the temperature of the raw synthesis gas discharged from the gasifier is not greater than 500 °C, or less than 400 °C, or not greater than 390 °C, or not greater than 375 °C, or not greater than 350 °C, or not greater than 325 °C, or not greater than 310 °C, or not greater than 300 °C, or not greater than 295 °C, or not greater than 280 °C, or not greater than 270 °C. The temperature of the raw synthesis gas leaving the gasification vessel is significantly lower than the temperature of the reaction product gas within the reaction zone. The temperature drop between the gasification zone gas temperature (or alternatively if more than one stage is used, all reaction zones) and the temperature of the raw synthesis gas discharged from the gasifier vessel can be at least 300 °C, or at least 400 °C, or at least 450 °C, or at least 500 °C, or at least 550 °C, or at least 600 °C, or at least 650 °C, or at least 700 °C, or at least 800 °C, or at least 900 °C, or at least 1000 °C, or at least 1050 °C, or at least 1100 °C.

[0462] As Figure 1 shown, the raw synthesis gas is discharged from the gasifier through line 16 to a suitable scrubber 17, where it contacts water from line 18 to remove remaining solid particles from the raw synthesis gas stream. The gas scrubber 17 can include a Venturi scrubber, a plate scrubber, or a packed tower or a combination thereof, where the raw synthesis gas stream is in close contact with water to achieve the removal of solid particles from the raw synthesis gas stream. The scrubbed raw synthesis gas stream is discharged through line 19 for further use in other processes, such as an acid gas (e.g., sulfur compounds) removal method to make the resulting purified synthesis gas stream suitable for chemical manufacture. Suitable methods for acid gas removal include Rectisol TMand Selexol TM A method for removing acid gases. Once sulfur substances are removed from the synthesis gas stream, elemental sulfur can be recovered and converted into sulfuric acid and other sulfur products, and the sulfur products can be commercialized by methods such as the Claus TM process.

[0463] As Figure 1 shown, the solid-water mixture from the gas scrubber 17 is discharged from the scrubber and optionally enters line 21 through line 20, where it is mixed with quenching water containing solids withdrawn from the quench zone 15 through line 22, and the mixture enters the settling tank 24 through the pressure reducing valve 23. The heat exchanger 25 is used to heat the relatively cold make-up water and recycled water by heat exchange with the hot cooling water from line 22, and the make-up water and recycled water are supplied from a suitable source through line 26 and pumped to the line for cooling and / or washing the product gas from the gas generator.

[0464] Solids including unreacted particulate coal settle out of the water in the settling tank 24 under the action of gravity and are withdrawn through line 27 as a concentrated slurry of ash, unreacted coal, and soot in water. The slurry can optionally be recycled via line 28 to the grinding zone 2. If desired, a portion of the slurry from line 27 can be transferred through line 29 to the mixing tank 6 to adjust the solids concentration in the water-coal-rubber slurry feed stream to the gasifier. Additionally, as Figure 2 shown, water and solids can be discharged from the settling tank 66 through line 83 for processing, while water and ash, unreacted coal, and soot can be discharged from the settling tank 66 through line 84 and mixed with the feedstock of coal, plastic, and water.

[0465] As Figure 1 shown, the gas released in the settler 24 can be discharged through line 30 and recovered as potential fuel gas. The clarified water from the settler 24 is discharged through line 31 and recycled to the quench water system through line 32. A portion of the water from line 32 is supplied to the quench zone 15 through line 33 after passing through the heat exchanger 25, and another portion of the water reaches the gas scrubber 17 through line 18. Additionally, water from the quench zone can be discharged to the settler 24 through line 22 via the control valve 23. The water level can be controlled by a level controller on the gasifier to maintain a substantially constant water level in the quench zone.

[0466] Alternatively or additionally, the quench water fed to the quench water zone through line 33 can be provided by a syngas scrubber downstream of the gasifier, as Figure 2 shown. The quench water stream that is optionally also fed to the quench zone can be clarified or can contain from about 0.1 wt.% to about 1.5 wt.% of soot, based on the weight of the quench water stream fed to the gasifier.

[0467] If desired, the high-temperature surfactant can be added directly to the quench water and enter the quench zone / compartment. Examples of such surfactants include any of the surfactants described above for stabilizing the feed stream, such as ammonium lignosulfonate or equivalent surfactants that are thermally stable at temperatures from about 300°F to about 600°F. Other surfactants include organic phosphates, sulfonates, and amine surfactants. The surfactant is used to establish a stable suspension of soot in the water at the bottom of the quench chamber, where the soot concentration can be at least 1 wt.%, or in the range from about 3.0 wt.% to about 15.0 wt.%, each based on the weight of the water in the quench chamber. The concentration of the active surfactant at the bottom of the quench zone can vary in the range from about 0.01 wt.% to about 0.30 wt.%.

[0468] In addition, as Figure 2 shown, an internal water jacket 79 is provided at the upper part of the quench zone 71 within the pressure vessel shell 50. The water jacket 79 prevents overheating of the pressure vessel shell below the height of the refractory 75 surrounding the reaction zone 54. Water is introduced into the water jacket 79 from line 80 and discharged therefrom via line 81 through valve 82, and can be fed directly or indirectly (via the settling tank 66) to the scrubber 59.

[0469] As Figure 1 shown, the slag and other heavy non-combustible solids that settle to the bottom of the quench zone 15 are periodically discharged as a water-solid slurry through line 34 and valve 35 into the lock hopper 36. The accumulated solid material from the lock hopper 36 is discharged through line 37 under the control of valve 38. In the operation of the lock hopper, during filling, valve 35 is open and valve 38 is closed, where the solid material from the quench chamber 15 is transferred to the lock hopper 36. Then valve 35 is closed, and the lock hopper 36 is emptied through line 37 by opening valve 38. The solid residue and water are discharged from the lock hopper 36 through line 37. Figure 2 Equivalent equipment and lines for the outlet 85, valves 86 and 88, line 89, and lock hopper 87 are shown in

[0470] In as Figure 1In an alternative embodiment, fresh water can be charged into the lock hopper 36 to displace the acidic water in the lock hopper 36. Cold clean water from line 39 is introduced into the lower part of the lock hopper 36 through valve 40. Valve 41 in line 42 is opened to establish communication between line 33 and the lock hopper 36. When the cold clean water enters the lower part of the lock hopper 36, the hot acidic water is discharged from the lock hopper and flows through line 42 and line 33 as part of the makeup water for the quench system into the quench zone 15. After the acidic water has been discharged from the lock hopper 36, valves 40 and 41 are closed, and valve 38 is opened to allow slag and clean water to be discharged from the lock hopper through line 37.

[0471] In an alternative embodiment, as Figure 1 shown, after the lock hopper has been charged with slag and acidic water from the quench zone 15 and valve 35 is closed, a stripping gas such as carbon dioxide or a gas produced by the gasifier (from which acidic gases have been removed by chemical treatment) can be introduced into the lower part of the lock hopper 36 through line 43. By opening valve 44 in line 43, the pressurized stripping gas is introduced into the lower part of the lock hopper 36. At the same time, valve 41 in line 42 is opened to allow the gas to enter the quench zone 15 through lines 42 and 33. The stripping gas from line 43 desorbs acidic gases, i.e., sulfides, cyanides, and other harmful gases, from the water in the lock hopper 36. When the desorbed gases are introduced back into the gasifier, they are mixed with the hot product gas and are discharged through line 16 as part of the product gas stream to the gas scrubber 17 for further purification and utilization after passing through the quench zone.

[0472] To illustrate one embodiment of the injector, reference is made to Figure 3 , which shows a partial cross-sectional view of a syngas gasifier at the injector location. The gasifier vessel includes a structural shell 90 and an internal refractory lining 91 (or linings) surrounding the enclosed gasification zone 93. Projecting outward from the shell wall is an injector mounting neck 94 for supporting the elongated fuel injector assembly 95 within the gasifier vessel. The injector assembly 95 is aligned and positioned such that the face 96 of the injector nozzle 97 is substantially flush with the inner surface of the refractory lining 91. The injector mounting flange 96 secures the injector assembly 95 to the mounting neck flange 97 of the gasifier vessel to prevent the injector assembly 95 from being ejected during operation. Oxygen feed flows into the central inner nozzle through pipe 98. The feedstock stream is fed to the injector assembly through line 99 and enters the annular space surrounding the central oxidizer nozzle. A cooling jacket surrounding the injector assembly 95 above the injector mounting flange 96 is supplied with cooling water 100 to prevent the injector assembly from overheating. Optional second oxidizer feed flows into the annular space through line 101, which surrounds at least a portion of the outer surface of the shell defining the feedstock ring.

[0473] Figure 4 A more detailed view of the injector is shown. A cross-sectional view of a portion of the injector assembly 80 toward the tip of the injector nozzle is shown. The injector assembly 80 includes an injector nozzle assembly 125, which includes three concentric nozzle housings and an external coolant jacket 110. The inner nozzle housing 111 discharges oxidant gas from an axial hole opening 112, and the oxidant gas is conveyed along Figure 3 the upper assembly axis conduit 98 in. The intermediate nozzle housing 113 guides the feed stream into the gasification zone 93. As a fluidized solid, the coal slurry is extruded from the annular space 114 defined by the inner wall 111 and the intermediate wall 113. The external oxidant gas nozzle housing 115 surrounds the external nozzle discharge ring 116. As Figure 3 shown, the upper assembly port 101 supplies an additional oxidizing gas stream to the external nozzle discharge ring. The centering fins 117 and 118 extend laterally from the outer surfaces of the inner nozzle housing wall 111 and the intermediate nozzle housing wall 113, respectively, to maintain coaxial centering of their respective housings relative to the longitudinal axis of the injector assembly. It can be understood that the structures of the fins 117 and 118 form a continuous band around the inner and intermediate housings and provide a small resistance to the fluid flow within the corresponding annular spaces.

[0474] To vary the flow rate, both the inner nozzle housing 111 and the intermediate nozzle housing 113 can be axially adjusted relative to the outer nozzle housing 115. When the intermediate nozzle 113 is axially displaced from the conical tapered inner surface of the outer nozzle 115, the outer discharge ring 116 is enlarged to allow a greater oxygen flow. Similarly, as the outer tapered surface of the inner nozzle 111 is axially pulled toward the inner conical surface of the intermediate nozzle 113, the feed slurry discharge area 114 is reduced.

[0475] Surrounding the outer nozzle housing 115 is a coolant fluid jacket 110 having an annular end cap 119. The coolant fluid conduit 120 conveys coolant, such as water, from Figure 3 the upper assembly supply port 100 in directly to the inner surface of the end cover plate 119. The flow channel baffle 121 controls the path of the coolant flow around the outer nozzle housing to ensure substantially uniform heat rejection and prevent coolant channeling and the generation of local hot spots. The end cap 119 includes a nozzle lip 122, which defines an outlet hole or discharge opening for feeding the reaction material into the injection injector assembly.

[0476] The planar end of the cooling sleeve 119 includes an annular surface 123 disposed facing the combustion chamber. Typically, the annular surface 123 of the cooling jacket is composed of a cobalt-based metal alloy material. Although cobalt is the preferred construction material for the nozzle assembly 125, other high-temperature melting point alloys such as molybdenum or tantalum may also be used. The heat shield 124 is formed of a high-temperature melting point material such as silicon nitride, silicon carbide, zirconia, molybdenum, tungsten, or tantalum.

[0477] Although this discussion is based on the injector and feed stream arrangements as described above, it should be understood that the injector may consist of only two channels for introducing and injecting the oxidizer and the feed stream, and they can be in any order, where the feed stream passes through the central axial hole opening while the feed passes through the annulus surrounding at least a portion of the central oxidizer duct, or the order can be reversed as described above.

[0478] An example of the operation of the gasifier and the scrubber is shown in Figure 2 . The coal / plastic feedstock slurry is fed into the gas generator 50 through an injector 51 mounted on top 52 of the gasifier and is fed together with oxygen through line 53 and is injected into the gasification zone 54 to produce raw syngas. The raw syngas discharged from the gasifier is fed into the contactor 55. Water is injected into the contactor 55 from line 56 through injectors 56 and 57. The intimate contact between the raw syngas from line 58 and the water from line 56 is desirably achieved through a venturi, nozzle, or orifice. In the contactor 55, the syngas stream is accelerated and water is injected into the accelerated gas stream from multiple injectors 56 and 57 at the throat of the nozzle, venturi, or orifice.

[0479] The resulting mixture of gas and water formed in the contactor 55 is directed into the scrubber 59 through a dip leg 60 that extends downward into the lower portion of the scrubber 59. The gas stream from the contactor 55 also carries entrained solid particles of unconsumed fuel or ash. A portion of the water is retained in the scrubber 59 and its water level can be controlled in any suitable manner, such as by the level controller 61 schematically shown. The dip leg 60 discharges the mixture of water and gas below the water level in the scrubber 59. By discharging the mixture of gas and water through the open end of the dip leg 60 into intimate contact with the water, the solid particles from the gas stream are trapped in the water.

[0480] The scrubber 59 is suitably in the form of a tower having an optional packing section 62 above the entry point of the gas stream from the contactor 55. Water from line 63 is introduced into the scrubber 59 above the height of the packing material 62. In the packing section 62, the gas stream comes into intimate contact with the water in the presence of a suitable packing material such as ceramic formed bodies, effecting substantially complete removal of solid particles from the gas stream. The product gas, which comprises carbon monoxide and hydrogen and contains water vapor, atmospheric gases and carbon dioxide, is discharged from the upper end of the scrubber 59 via line 64, its temperature corresponding to the equilibrium evaporation temperature of water at the pressure prevailing in the scrubber 59. The clean synthesis gas from line 64 can be further processed, for example, for the production of a higher concentration of hydrogen by the water-gas shift reaction and suitable downstream purification to remove sulfur.

[0481] Water from the lower part of the scrubber 59 enters the injectors 56 and 57 via line 56 by means of a pump 65. Clarified water from the settler 66 can also be supplied to line 56 via line 68 by means of a pump 67. Water is discharged from the scrubber 59 by means of a pump 69 and passes through a valve 70 responsive to the level controller 61 on the scrubber and via line 72 into the quench zone 71 to control the level in the scrubber 59.

[0482] Any heavy solid particles removed from the gas stream in the downcomer 60 settle into the water slurry, are collected in the water bath at the bottom of the scrubber 59 and are discharged at periodic intervals at the bottom pipe 73 via line 74 under the control of a valve 75.

[0483] Any suitable scrubber design can be used in the process. Other scrubber designs include plate-type contact towers in which the gas contacts the water in countercurrent. The water is introduced into the scrubber at a location near the top of the tower.

[0484] Example

[0485] Example 1

[0486] The plastic is ground to a nominal particle size between 1 mm and 0.5 mm. The coal is dried and crushed to a nominal size <2 mm in a Retsch jaw crusher. A predetermined amount of water is added to a 4.5 L metal bucket. Ammonium lignosulfonate is added to the water in the metal bucket and mixed with a spatula until it is evenly distributed. The ground plastic and coal are added to the water and ALS mixture in the metal bucket and the blend is then mixed by an overhead mixer. Ammonia water is added to the slurry to adjust the pH to 8 ± 0.2. After thorough mixing, the sample is placed in a laboratory rod mill equipped with 5 1 / 2 ”X 9” stainless steel rods, 8 pieces of 5 / 8” X 9” stainless steel rods, 8 pieces of “ 3 / 4 Stainless steel bars of "X 9", 2 stainless steel bars of "1" X 9", and 1 1 / 4 stainless steel bar of "X 9". Grind the slurry at about 28 rpm (mill outer diameter = 11.75 inches) for 1 hour. When mixing the slurry through the top tower mixer, adjust the pH to 8 ± 0.2 again using ammonia water. Each batch of slurry is made to a total of about 3000 grams, has about 69% solids, and has different amounts of recycled materials as shown in Table 1 below. The results of the viscosity and stability tests are listed in Table 1.

[0487] Transfer a 500 - 550 g coal slurry sample to a 600 mL glass beaker to measure viscosity and stability. The stability of each sample can be judged by visual inspection. Mix the slurry well to produce a uniform distribution of particles throughout the sample and let the slurry stand undisturbed for a period of time. Then remix the slurry. If a layer of particles separates at the bottom of the beaker, the slurry will be difficult to remix and is subsequently considered to have settled. After some time, the slurry will have settled. However, the longer the amount of time required for settlement, the better, medium, or poor the stability of the slurry is determined to be. If the slurry settles before 5 minutes, it is considered poor.

[0488] In an alternative method, the stability of the slurry can be quantitatively determined. At room temperature, measure the viscosity of the slurry sample using a Brookfield viscometer with an LV - 2 spindle rotating at a rate of 0.5 rpm (Method A) or a Brookfield R / S rheometer with a V80 - 40 vane spindle operating at a shear rate of 1.83 / S (Method B). Report the average of 3 viscosity measurements.

[0489] By Method A or Method B, after the slurry is well - mixed to form a uniform distribution of solids, measure the stability by dipping the spindle of the rheometer into the slurry at the bottom of the beaker. After a specified period of time, measure the viscosity with the spindle at the bottom of the beaker. The viscosity increases with settlement, and if the initial reading at the start of the viscosity measurement is 100,000 cP, the slurry is considered to have settled. Thus, if the initial viscosity is 100,000 cP or less after standing for 5 minutes, the slurry is considered stable.

[0490] If the viscosity reading is 30,000 cP or less (desirably 25,000 cP or less or preferably 20,000 cP or less) when taking a reading immediately after the slurry is well - mixed to form a uniform distribution of solids, the slurry is considered pumpable.

[0491] The results of stability were determined visually, and the results of pumpability were recorded in the viscosity column for Method A in Table 1. The ground plastic was the original PET pellets, ground to a nominal size of 1 mm or less. Stability was determined at the 5-minute mark.

[0492] Table 1 - Effect of increased ground plastic loading on coal-water slurry properties.

[0493]

[0494]

[0495] a Measured by Method A.

[0496] Up to 61.7% solids (26.2% of the total slurry) of the mixtures for all tests exhibited good slurry properties and were suitable for use in a gasifier. At low loadings, the stability of the slurry was good.

[0497] Example 2

[0498] As described in Example 1 and in the amounts reported in Table 2, batches of coal / plastic slurries were prepared using low density polyethylene as the plastic. The results of stability and pumpability using Method B in each case were recorded in Table 2 below. A "stable" report in the stability column indicates a viscosity reading of less than 100,000 cP over the period stated.

[0499] Table 2 - Effect of increased ground LDPE loading on coal-water slurry properties.

[0500]

[0501] All samples remained stable for 5 minutes. However, at a solids loading of 10%, the LDPE samples were considered too thick to pump effectively.

[0502] Example 3

[0503] All recycled plastics were reduced in size and ground so that they passed through a 1.5 mm screen. Batches of coal / recycled plastic slurries were prepared using various different types of plastics as described in Example 1 and in the amounts reported in Table 2, according to the following instructions. The results of stability and pumpability using Method B in each case were recorded in Table 2 below.

[0504] The following legend describes the plastics used:

[0505] PEX: Cross-linked polyethylene

[0506] LDPE Low density polyethylene

[0507] PET Polyethylene terephthalate

[0508] CDA: Cellulose diacetate

[0509] DEP: Diethyl phthalate

[0510] HDPE: High-density polyethylene

[0511] Cellulose tow: Cellulose acetate tow:

[0512]

[0513]

Claims

1. A method for producing syngas, comprising: a. charging an oxidant and a feedstock composition into a gasification zone within a gasifier, said feedstock composition comprising a solid fossil fuel, and up to 15 wt.% recycled plastic, based on the weight of the solids in the feedstock composition; b. gasifying said feedstock composition with said oxidant in the gasification zone to produce a syngas composition; and c. discharging at least a portion of said syngas composition from said gasifier; wherein said gasifier is a entrained flow gasifier, and wherein, (i) the amount of CO2 produced by a stream of recycled plastic and solid fossil fuel (mixed stream) is not greater than 25% of the amount of carbon dioxide produced by a stream of only fossil fuel, where the amount of recycled plastic in the stream of only fossil fuel is replaced with said solid fossil fuel, or (ii) the carbon monoxide / hydrogen ratio produced by a stream of recycled plastic and solid fossil fuel (mixed stream) is within 10% of the carbon monoxide / hydrogen ratio produced by the same stream with the recycled plastic content replaced with the same solid fossil fuel, or (iii) both of the above.

2. The method according to claim 1, wherein, 90 wt.% of said recycled plastic has a particle size not greater than 2 mm in the maximum dimension.

3. The method according to claim 2, wherein, at least one of the following conditions exists: (i) the gasification in said gasification zone is carried out at a temperature of at least 1000 °C, or (ii) the pressure in said gasification zone is greater than 2.7 MPa, or (iii) said feedstock composition is a slurry, or (iv) no steam is introduced into said gasifier and flows into said gasification zone, or (v) said recycled plastic is pre-ground such that at least 90% of the particles have a particle size less than 2 mm, or (vi) the tar yield is less than 4 wt.%, or (vii) said gasifier does not contain a membrane wall in said gasification zone, or (viii) a combination of two or more of the above conditions.

4. The method according to claim 1, comprising a syngas composition stream having a switching variability of negative, zero or not greater than 15%, where the switching frequency is at least 1x / 2 years and the switching variability is determined by the following equation: where %SV is the percentage of syngas switching variability of one or more measured components in said syngas composition; and V m is the syngas compositional variability of gaseous compounds using a mixed stream comprising recycled plastics and fossil fuels; and V ff is the syngas compositional variability of the same gaseous compounds of a stream using only fossil fuels, and wherein the solid concentration is the same in both cases, the fossil fuels are the same in both cases, and the feedstock is gasified under the same conditions, except for possible temperature fluctuations that are different in themselves due to having recycled plastics in the feedstock, and the variability is measured and meets at least one of the following gaseous compounds (in moles): a. the amount of CO, or b.H 2 quantity, or c. the amount of CO2, or d. the amount of CH4, or e. the amount of H2S, or f. the amount of COS, or g. the amount of H2 + CO, or its sequential molar ratio (e.g., H2:CO ratio), or h. the amount of H2 + CO + CO2, or its sequential molar ratio, or i. the amount of H2 + CO + CH4, or its sequential molar ratio, or j. the amount of H2 + CO + CO2 + CH4, or its sequential molar ratio, or k. the amount of H2S + COS, or its sequential molar ratio, or l.H2+CO+CO 2 +CH 4 +H 2 S+COS。 5. The method according to claim 1, wherein, said plastic is pre-ground before being added to said fossil fuel.

6. The method according to claim 1, wherein, at least 80 wt.% of all feedstocks other than the solid fossil fuel in the feedstock stream fed to said gasifier is plastic.

7. The method according to claim 1, wherein, the feed stream contains less than 1 wt.% of added liquid fractions from refined crude oil or reformed any such fractions, based on the weight of the feed stream, and wherein no gas stream contains more than 0.03 mole%.

8. The method according to claim 1, wherein, the feed stream is not introduced into the side wall of the gasifier and the gasifier does not include a tangential feed injector, and the oxidizer and the feed stream are fed in co-current, and wherein the feed stream is not processed through a lock hopper or pressurized in a lock hopper before entering the injector or entering the gasification zone.

9. The method according to claim 1, wherein, operating the gasifier under conditions for forming slag in the gasification zone, the gasifier being a down-flow reactor and the flow of the synthesis gas being vertically downward, and the gasifier being a single-stage reactor, and the position where the synthesis gas stream is withdrawn from the gasifier is lower than at least one position where the feed stream is introduced.

10. The method according to claim 1, wherein, incorporating the granulated plastic into the feed stream is continuous for at least 1 day (24 hours), the gasification zone and optionally all reaction zones are operated at a temperature greater than 1000 °C and up to about 1800 °C, or the gasifier is operated at a pressure of at least 400 psig (2.76 MPa) in the gasification zone (or combustion chamber).

11. The method according to claim 1, wherein, no portion of the synthesis gas discharged from the gasifier is used to heat the gasifier or burned to dry the solid fossil fuel.

12. The method according to claim 1, wherein, the pre-ground plastic includes cellulose, or comprises a copolyester having a plurality of cyclohexanedimethanol moieties, 2,2,4,4-tetramethyl-1,3-cyclobutanediol moieties, or includes low density polyethylene, high density polyethylene, linear low density polyethylene, polypropylene, polymethylpentene, polybutene-1, and their copolymers or combinations thereof.

13. The method according to claim 1, wherein, the pre-ground plastic includes pre-ground plastic obtained from spectacle frames, cross-linked polyethylene tubes, flash-spun high density polyethylene or combinations thereof.

14. A method for producing a synthesis gas composition, comprising: a. charging an oxidizer and a feed composition comprising recycled plastic and solid fossil fuel into a gasification zone within a gasifier; b. gasifying the feed composition with the oxidizer in the gasification zone to produce the synthesis gas composition; and c. discharging at least a portion of the synthesis gas composition from the gasifier; wherein the recycled plastic is added to the solid fossil fuel at a feed point, the feed point including a solid fossil fuel conveyor belt feeding the grinder after the solid fossil fuel is loaded onto the conveyor belt, a solid fossil fuel conveyor belt feeding the grinder before the solid fossil fuel is loaded onto the conveyor belt, or a solid fossil fuel slurry storage tank containing the solid fossil fuel ground to a size the same as that fed to the gasification zone, and wherein, (i) The amount of CO2 produced from a stream of recycled plastic and solid fossil fuel (mixed stream) is no greater than 25% of the amount of carbon dioxide produced from a stream of fossil fuel only, where the amount of recycled plastic in the stream of fossil fuel only is replaced with the solid fossil fuel, or (ii) The ratio of carbon monoxide / hydrogen produced from a stream of recycled plastic and solid fossil fuel (mixed stream) is within 10% of the ratio of carbon monoxide / hydrogen produced from the same stream with the recycled plastic content replaced with the same solid fossil fuel, or (iii) Both of the above.

15. A feedstock slurry composition comprising recycled plastic, solid fossil fuel, and water, wherein the recycled plastic has a particle size of no greater than 2 mm, and the solid fossil fuel in the feedstock composition has a particle size of less than 2 mm, the solid content in the slurry is at least 62 wt.%, the amount of recycled plastic present in the feedstock slurry composition is at least 0.1 wt.% and at most 25 wt.%, based on the weight of all solids, and the amount of water is at least 20 wt.%, based on the weight of the feedstock slurry composition, and wherein: a. The slurry is stable, as determined using a Brookfield R / S rheometer operating at a shear rate of 1.83 / s equipped with V80 - 40 blades or a Brookfield viscometer with an LV - 2 spindle rotating at a rate of 0.5 rpm, having an initial viscosity of 100,000 cP or less at 5 minutes, measured under ambient conditions; or b. The slurry is pumpable, as determined after mixing to obtain a uniform distribution of solids throughout the slurry and using a Brookfield R / S rheometer operating at a shear rate of 1.83 / s equipped with V80 - 40 blades or a Brookfield viscometer with an LV - 2 spindle rotating at a rate of 0.5 rpm or a Brookfield R / S rheometer operating at a shear rate of 1.83 / s equipped with V80 - 40 blades or a Brookfield viscometer with an LV - 2 spindle rotating at a rate of 0.5 rpm or a Brookfield R / S rheometer operating at a shear rate of 1.83 / s equipped with V80 - 40 blades or a Brookfield viscometer with an LV - 2 spindle rotating at a rate of 0.5 rpm, having a viscosity of less than 30,000 cP, measured under ambient conditions, or c. Both of the above; and wherein, (i) The amount of CO2 produced from a stream of recycled plastic and solid fossil fuel (mixed stream) is no greater than 25% of the amount of carbon dioxide produced from a stream of fossil fuel only, where the amount of recycled plastic in the stream of fossil fuel only is replaced with the solid fossil fuel, or (ii) The ratio of carbon monoxide / hydrogen produced from a stream of recycled plastic and solid fossil fuel (mixed stream) is within 10% of the ratio of carbon monoxide / hydrogen produced from the same stream with the recycled plastic content replaced with the same solid fossil fuel, or (iii) Both of the above.

16. A syngas composition that is discharged from a gasifier and obtained by gasifying a feed stream comprising recycled plastics and solid fossil fuels, wherein (i) the amount of the recycled plastics is at most 25 wt.%, based on the solid weight in the feed stream, or (ii) the recycled plastics have a particle size not greater than 2 mm, or (iii) both of the above, and the syngas stream does not contain tar or contains less than 4 wt.% of tar, based on the weight of all condensable solids in the syngas composition.

17. Use of plastics in the production of syngas by gasifying a slurry of plastics and solid fossil fuels in a entrained flow gasifier under slagging conditions.

18. A syngas combined stream that is produced by gasifying a feedstock (mixed feed) comprising solid fossil fuels and recycled plastics in a gasifier, the feedstock having a compositional variability of 5% or less measured over a period of 12 days or the shorter of the periods during which the mixed feed is fed to the gasifier, and the syngas compositional variability is measured and meets at least one of the following gaseous compounds (in moles): a. The amount of CO, or b. The amount of H2, or c. The amount of CO2, or d. The amount of CH4, or e. The amount of H2S, or f. The amount of COS, or g. The amount of H2 + CO, or its sequential molar ratio (e.g., H2:CO ratio), or h. The amount of H2 + CO + CO2, or its sequential molar ratio, or i. The amount of H2 + CO + CH4, or its sequential molar ratio, or j. The amount of H2 + CO + CO2 + CH4, or its sequential molar ratio, or k. The amount of H2S + COS, or its sequential molar ratio, or l.H2+CO+CO 2 +CH 4 +H 2 S+COS。

Citation Information

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