Supply mixing device

Abstract

The present invention relates to a feed mixing device for particles that can be injected into a reactor, such as a co-flow reactor. Thus, it is possible to utilize the deaggregated particles in the reactor. For example, deaggregation allows for rapid heating of the particles, which is beneficial for, for example, the formation of carbon black.

Description

[Technical Field]

[0001] The present invention relates to a feed mixing device for particles that can be injected into a reactor, such as a co-flow reactor. Thus, it is possible to utilize the deaggregated particles in the reactor. For example, deaggregation allows for rapid heating of the particles, which is beneficial for, for example, the formation of carbon black. [Background technology]

[0002] The use of particles in reactors is difficult to implement. Particles tend to aggregate, reducing their specific surface area. However, a high specific surface area is often required for particles to be utilized in chemical reactions.

[0003] It is particularly desirable to provide apparatus and methods for utilizing particle or particulate carbon-containing raw materials for the production of carbon black.

[0004] Carbon black has many applications, such as a reinforcing or filler for the rubber and tire industries. Furthermore, its use is increasing in other areas, such as a colorant and toner for photocopiers. The diverse applications of carbon black require a wide range of properties, including particle size, structure, yield, surface area, and dyeability. Carbon black formation can be separated into different process steps, including raising the temperature of the raw materials to the thermal decomposition temperature, thermal decomposition of the raw materials into unsaturated species such as acetylene and aromatic intermediate products, nucleation, surface growth, and aggregation.

[0005] However, the raw materials used to produce carbon black must be converted into gaseous components before thermal decomposition. Liquid raw materials are generally used in carbon black production because they evaporate significantly faster than particulate raw materials. While particles with small diameters can be used, these often exist as aggregates. Since aggregated particles heat up slowly, their evaporation may be insufficient.

[0006] Therefore, it is desirable that the particles be utilized within a reactor, preferably a furnace reactor. The present invention provides a feed mixing device for particles. The particles are deaggregated by utilizing an accelerated carrier gas flow.

[0007] De-aggregated particulate carbon-containing raw materials have been shown to be usable in the production of carbon black. [Overview of the Initiative]

[0008] The objective is achieved by a device for supplying and mixing particles into a reactor, the supply-mixing device comprising: (i) a carrier gas passage extending through the supply-mixing device; (ii) at least one carrier gas inlet fluidly communicating with the carrier gas passage; (iii) at least one particle inlet; (iv) a mixing chamber fluidly communicating with the at least one particle inlet and the carrier gas inlet; (v) a deagglutinating conduit fluidly communicating with the mixing chamber; (vi) at least one outlet for the carrier gas encompassing the particles supplied to the mixing chamber, the at least one outlet fluidly communicating with the deagglutinating conduit; and (vii) means for accelerating and injecting the carrier gas flow into the mixing chamber.

[0009] Furthermore, a reactor system is provided which includes a reactor and a feed mixing device according to the present invention, wherein the feed mixing device is in fluid communication with the reactor.

[0010] Furthermore, a method for injecting particulate matter into a reactor, comprising the steps of (a) deaggregating and entraining the particles into a carrier gas stream, preferably by using a feed mixing device according to the present invention, and (b) injecting the carrier gas stream containing the deaggregated particles obtained in step (a) into the reactor.

[0011] Furthermore, the supply and mixing apparatus according to the present invention is used to deaggregate particles, preferably particulate carbon-containing raw materials. [Brief explanation of the drawing]

[0012] [Figure 1] Cross-section of a furnace reactor

[0013] [Figure 2] Feed mixing device with nozzle

[0014] [Figure 3] Laval nozzle for feed mixing device

[0015] [Figure 4] Deagglutination conduit for supply mixing device [Modes for carrying out the invention]

[0016] As used herein and in the appended claims, the singular forms “a,” “an,” and “the” include multiple referents unless the context clearly indicates otherwise. Thus, for example, a reference to “oxygen-containing gas” includes mixtures of oxygen-containing gases, and a reference to “fuel” includes mixtures of two or more such fuels, and so on.

[0017] Unless otherwise specified, diameter always refers to the inner diameter of an object. For example, the diameter of a tubular conduit refers to the inner diameter of the tubular conduit.

[0018] The term "raw material" refers to the raw materials supplied for the manufacture of carbon black. Particulate raw materials can be used in the manufacture of carbon black. As used herein, the term or abbreviation "raw material" refers to particulate carbon-containing raw materials. Particulate raw materials may contain up to 10% by weight of oil (bulking oil). For example, rubber granules often contain up to 10% by weight of oil (bulking oil). The oil or bulking oil is generally an aliphatic oil or an aromatic oil.

[0019] The term "high-temperature gas flow" refers to the carrier gas in an accompanying flow reactor, such as a furnace reactor, which heats the reaction mixture (including particulate carbon-containing raw materials) to the temperature required for the thermal decomposition reaction. For example, a "high-temperature gas flow" is the gas flow after the combustion of fuel in a furnace reactor.

[0020] As used herein, “carbon black” means a material consisting substantially of more than 80% by weight, 90% by weight, or 95% by weight, of carbon, based on total weight, produced by the thermal decomposition of carbon-containing raw materials or radical-driven extraction of non-carbon atoms. Various industrial methods for producing carbon black are known, including furnace processes, gas black processes, acetylene black processes, thermal black processes, or lamp black processes. The production of carbon black is well known in the art and is outlined, for example, in J.-B. Donnett et al., “Carbon Black: Science and Technology,” 2nd edition, so it will not be described in further detail here.

[0021] The reaction volume of the reactor is the volume of the reactor between the injection point of the particulate carbon-containing raw material and the quenching point.

[0022] A device for supplying and mixing particles into a reactor, comprising: (i) a carrier gas passage extending through a supply mixer; (ii) at least one carrier gas inlet in fluid communication with the carrier gas passage; (iii) at least one particle inlet; (iv) a mixing chamber in fluid communication with at least one particle inlet and the carrier gas inlet; (v) a deagglutinating conduit in fluid communication with the mixing chamber; (vi) at least one outlet for carrier gas accompanying particles supplied into the mixing chamber, the at least one outlet in fluid communication with the deagglutinating conduit; and (vii) means for accelerating and injecting a carrier gas flow into the mixing chamber.

[0023] A preferred supply and mixing apparatus is shown in Figure 2.

[0024] The gas passage should extend along the longitudinal axis of the supply mixing device, and preferably the at least one inlet, mixing chamber, deagglutination conduit, and outlet are located along the longitudinal axis.

[0025] The deagglutinating conduit is preferably a tubular deagglutinating conduit.

[0026] The particle inlet should be configured to supply particles into the mixing chamber at an angle to the carrier gas injection released into the mixing chamber, preferably perpendicular to the carrier gas injection. However, the angle is not particularly limited in this invention.

[0027] The means for accelerating and injecting the carrier gas flow may include at least one injection nozzle (nozzle). The injection nozzle is configured to accelerate the carrier gas flow. This means that the nozzle (or injection nozzle) is positioned such that it converges in the direction of flow so that the gas flow is accelerated after it leaves the nozzle and enters the mixing chamber. In other words, the means for accelerating and injecting the carrier gas flow preferably converges in the direction of flow extending from the at least one carrier gas inlet toward the at least one outlet.

[0028] The injection nozzle may be a Laval nozzle. Such a Laval nozzle (or nozzle) may include a converging section, a throat, and a diverging section (in the following order). Typically, the converging section reduces the diameter of the nozzle so that the gas flow is accelerated. The diverging section increases the diameter of this section. However, the diameter increased by the diverging section is still smaller than the diameter before the converging section. Therefore, a nozzle including a converging section, a throat, and a diverging section accelerates the gas flow in the following order.

[0029] The cross-sectional area is typically circular or elliptical at each point of the spray nozzle.

[0030] The spray nozzle may include a diverging section, the angle of which can be 2 to 30°, preferably 3 to 20°, more preferably 4 to 15°, and most preferably 5 to 10°.

[0031] The injection nozzle may include a converging section, the maximum inner diameter of which can be 5 to 50 mm, preferably 8 to 40 mm, more preferably 10 to 30 mm, and most preferably 12 to 20 mm.

[0032] The minimum inner diameter of the converging and diverging sections and / or the inner diameter of the throat can be 0.6 to 30 mm, preferably 1.2 to 18 mm, more preferably 1.9 to 12 mm, and most preferably 3 to 9 mm.

[0033] The minimum inner diameters of the converging and diverging sections, as well as the inner diameter of the throat, should be the same. In other words, the converging section, throat, and diverging section are generally directly connected to one another.

[0034] The spray nozzle may include a diverging section, the maximum inner diameter of which can be 0.3 to 11 mm, preferably 0.5 to 7 mm, more preferably 0.9 to 5 mm, and most preferably 1.1 to 4 mm.

[0035] The minimum inner diameter of the converging section must be greater than the maximum inner diameter of the converging section, preferably the difference between the maximum inner diameters of the converging and diverging sections is 5 to 30 mm, preferably 8 to 20 mm, more preferably 9 to 18 mm, and most preferably 10 to 15 mm.

[0036] The maximum inner diameter of the converging section may be greater than the maximum inner diameter of the diverging section.

[0037] The distance between the accelerating and injecting means and the conduit having a certain inner diameter can be 2 to 20 mm, preferably 2.5 to 15 mm, more preferably 3 to 10 mm, and most preferably 3.5 to 7 mm. The specific distance between the aforementioned components improves the deagglomeration of particles because the jet flows directly into the deagglomeration conduit. Thus, turbulence can be avoided and the velocity loss of the jet flow can be minimized.

[0038] The means (or nozzle) for accelerating and injecting the carrier gas may be positioned such that the means for accelerating and injecting the carrier gas protrudes into the cavity of the inlet funnel of the deagglutination conduit.

[0039] Deagglutination conduits typically include conduits with a fixed inner diameter. In conduits with a fixed inner diameter, particles further deagglutinate by colliding with each other or by colliding with the walls of the conduits with a fixed inner diameter. Deagglutination conduits can be configured as diffusion tubes.

[0040] The deagglutination conduit may include an inlet funnel, a conduit with a constant inner diameter, and a diffusion nozzle that extends in the direction of flow, from downstream to upstream. The diffusion nozzle should continuously increase the inner diameter of the deagglutination conduit. Therefore, the carrier gas flow is not interrupted and turbulence is avoided. The angle of the diffusion nozzle can be 1 to 30°, preferably 2 to 20°, more preferably 3 to 15°, and most preferably 4 to 8°. The angle of the inlet funnel can be 20 to 80°, preferably 30 to 75°, more preferably 40 to 70°, and most preferably 50 to 65°.

[0041] The longitudinal axis of the deagglutination conduit can be coaxial with the longitudinal axis of the feed mixing device. Coaxial arrangement improves overall acceleration and deagglutination.

[0042] The inner diameter of a conduit having a certain inner diameter can be 1 to 20 mm, preferably 2 to 10 mm, more preferably 3 to 7 mm, and most preferably 4 to 6 mm. The inner diameter can affect deagglomeration. Therefore, the diameter should be selected for a specific raw material, preferably for a mass flow rate.

[0043] The maximum inner diameter of the diffusion nozzle is greater than the inner diameter of a conduit having a constant inner diameter. The maximum inner diameter of the diffusion nozzle should be 5 to 50 mm, preferably 8 to 40 mm, more preferably 10 to 30 mm, and most preferably 12 to 20 mm.

[0044] The focusing sections of the diffusion nozzle and the injection nozzle can have the same maximum inner diameter.

[0045] The maximum inner diameter of the diffusion nozzle can be 5 to 50 mm, preferably 8 to 40 mm, more preferably 10 to 30 mm, and most preferably 12 to 20 mm.

[0046] The length of the conduit having a certain inner diameter can be 3 to 500 mm, preferably 5 to 200 mm, more preferably 10 to 50 mm, and most preferably 13 to 30 mm. The length of the conduit can have a beneficial effect on the deaggregation of particles (particulate carbon-containing raw material). Longer conduits generally result in better deaggregation.

[0047] The length of the diffusion nozzle can be 10 to 300 mm, preferably 20 to 200 mm, more preferably 25 to 150 mm, and most preferably 30 to 100 mm.

[0048] The inner diameter of a conduit having a certain inner diameter must be greater than the maximum inner diameter of the outlet of the means for accelerating and injecting the carrier gas flow.

[0049] The means for accelerating and injecting the carrier gas flow, the mixing chamber, and the deagglutination conduit should be configured such that the carrier gas injection is discharged into the deagglutination conduit.

[0050] The supply mixing device may further include at least one hopper upstream of the at least one particle inlet.

[0051] At least one screw conveyor, such as a screw conveyor, is often located upstream of at least one particle inlet. The screw conveyor should be configured to supply a certain amount of particles (or particulate carbon-containing material) into the mixing chamber. Thus, the particle supply can be controlled by the screw conveyor.

[0052] The particles described herein are typically particulate carbon-containing raw materials, and the reactor is typically a co-flow reactor for carbon black production.

[0053] The supply and mixing often further includes a pressure tank for particles, which is in fluid communication with at least one particle inlet and at least one optional screw conveyor. Preferably, two pressure tanks are present, with the first pressure tank connected to the second pressure tank. Both pressure tanks can be connected via valves.

[0054] A reactor system can be provided that includes a co-flow reactor and a feed mixer, the feed mixer being in fluid communication with the reactor. The feed mixer should preferably be connected to multiple inlets of the reactor by injection lances.

[0055] The feed mixing device can be fluidly connected to a tunnel upstream of the choke, combustion chamber, and / or the quenching region of the co-flow reactor. The reactor can be a co-flow reactor, preferably a furnace reactor.

[0056] A method for injecting particulate matter into a reactor is provided, comprising the steps of (a) deaggregating and entraining the particles in a carrier gas stream, preferably by using a feed mixing device according to the present invention, and (b) injecting the carrier gas stream containing the deaggregated particles obtained in step (a) into the reactor.

[0057] This method may be a method for producing carbon black, the particulate material may be a particulate carbon-containing raw material, and the reactor may be a co-flow reactor for producing carbon black, preferably a furnace reactor.

[0058] The particulate carbon-containing raw material can be injected into the co-flow reactor through multiple inlets, preferably through multiple injection lances.

[0059] The carrier gas flow can be accelerated and flow through the mixing chamber into the deagglutination conduit.

[0060] Deagglutination can be performed by accelerating particles in a carrier gas stream and causing them to collide with the inner surface of a deagglutination conduit.

[0061] The carrier gas is generally accelerated to 1 Ma or more, preferably 1.01 Ma to 1.7 Ma, more preferably 1.1 Ma to 1.6 Ma, and most preferably 1.2 Ma to 1.5 Ma. However, flow velocities of 0.01 Ma to 3 Ma, preferably 0.1 Ma to 2 Ma, more preferably 0.2 to 1.8 Ma, and most preferably less than 0.3 to 1 Ma are also desirable. Ma is the Mach number.

[0062] The particles can be directed perpendicularly to the carrier gas injection and used for the carrier gas injection.

[0063] The carrier gas stream containing the deaggregated particles can be injected into the reactor at a pressure of 0.5 bar to 2 bar, preferably 0.7 bar to 1.5 bar, more preferably 0.8 to 1.3 bar, and most preferably 0.8 to 1.2 bar. The pressure should be adjusted according to the injection position of the feedstock. For example, the pressure in the combustion chamber is higher than the pressure in the choke, and as a result, the deaggregated particulate carbon-containing feedstock, or the carrier gas containing the deaggregated particulate carbon-containing feedstock, should be injected into the combustion chamber at a higher pressure.

[0064] The carrier gas may further contain H2O and / or additives. The carrier gas may contain 1 to 10 volume percent of H2O. H2O can prevent particle re-aggregation.

[0065] The supply and mixing device can be used to deaggregate particles, preferably particulate carbon-containing raw materials.

[0066] It is particularly preferable that the particulate carbon-containing raw material be deaggregated before injection into the reactor. The evaporation time is expected to be reduced by using deaggregated particles.

[0067] Acceleration of particulate carbon-containing raw materials leads to deaggregation of the particles. For example, a carrier gas such as N2 or air can be accelerated, and the particles can be injected into the accelerated carrier gas. In other words, deaggregation can be carried out by subjecting the particulate carbon-containing raw material to carrier gas injection.

[0068] Deagglutination can be performed (i) in a feed mixing device including a Laval nozzle.

[0069] Deaggregation can also be achieved by collisions between accelerated particulate carbon-containing material and an object (such as two particles of particulate carbon-containing material), or by collisions between particles and a surface, such as the inner surface of a deaggregation conduit.

[0070] The deagglomerated particulate carbon-containing raw material can be contained in a carrier gas, which may further contain H2O and / or additives. H2O can prevent the re-agglomeration of particles in the carrier gas. Therefore, the deagglomerated particulate carbon-containing raw material should be contained in a carrier gas, which may further contain 1 to 10 volume%, preferably 2 to 8 volume%, and more preferably 3 to 7 volume%, of H2O based on the total volume of the carrier gas containing the deagglomerated particulate carbon-containing raw material.

[0071] Particulate carbon-containing raw materials and / or de-aggregated carbon-containing raw materials are generally contained in or entrained in the carrier gas.

[0072] A method for producing carbon black from particulate carbon-containing raw materials in a co-flow reactor having a flow channel along the central longitudinal axis of the reactor may include (a) providing a high-temperature gas flow, (b) providing particulate carbon-containing raw materials, and (d) injecting the particulate carbon-containing raw materials into the high-temperature gas flow to form carbon black, wherein the high-temperature gas flow has a temperature of at least 800°C.

[0073] While not bound by theory, since the heating rate of particulate carbon-containing feedstock is lower compared to liquid carbon-containing feedstock, it is desirable that the particulate carbon-containing feedstock be injected into the high-temperature gas flow of the co-flow reactor at a suitable temperature of 800°C or higher. For example, the temperature of the high-temperature gas flow can be at least 900°C, at least 1000°C, at least 1100°C, at least 1200°C, at least 1300°C, at least 1400°C, at least 1500°C, or at least 1600°C. The desired minimum temperature can be determined by measuring the transmittance of the produced carbon black. If the transmittance is low, the temperature of the high-temperature gas flow can be increased.

[0074] High-temperature gas flows can be obtained by electric preheating, plasma heating, and combustion of fuel and oxygen-containing gases. High-temperature gas flows can be provided by (a1) supplying fuel and oxygen-containing gases into the combustion chamber of a reactor, and (b2) burning the fuel in the combustion chamber to generate a high-temperature gas flow.

[0075] Therefore, a method can be provided for producing carbon black from particulate carbon-containing raw materials in a co-flow reactor having a flow path along the central longitudinal axis of the reactor, comprising (a) supplying fuel and oxygen-containing gas into the combustion chamber of the reactor, (b) burning the fuel in the combustion chamber to generate a high-temperature combustion gas, and (d) injecting particulate carbon-containing raw materials into the high-temperature gas flow to form carbon black, wherein the high-temperature combustion gas has a temperature of at least 800°C.

[0076] As described above, the particles may include particulate carbon-containing raw materials. Particulate carbon-containing raw materials may include inert compounds, coke, C,H-containing compounds, and / or carbon black, preferably carbon black and C,H-containing compounds. Typically, particulate carbon-containing raw materials are particles, generally aggregated particles. In contrast, liquid carbon-containing raw materials mean that the raw material is liquid at 20°C and 1 atmosphere. In methods for producing carbon black, it is preferable not to use liquid carbon-containing raw materials in the production of carbon black.

[0077] Generally, the raw materials used in carbon black production are particulate carbon-containing materials.

[0078] Particulate carbon-containing raw materials are suitable raw materials for producing carbon black, i.e., new carbon black. Therefore, particulate carbon-containing raw materials contain materials that can be thermally decomposed.

[0079] C,H-containing compounds (hydrocarbon compounds) can be used to produce carbon black, i.e., new carbon black (nCB) or virgin carbon black (vCB). C,H-containing compounds refer to compounds containing C and H, respectively. For example, C,H-containing compounds are hydrocarbon compounds that can contain heteroatoms such as O or S.

[0080] The particulate carbon-containing raw material may contain 10 to 100% by weight of C,H-containing compounds, preferably 20 to 99% by weight of carbon and hydrogen-containing compounds, more preferably 30 to 90% by weight of carbon and hydrogen-containing compounds, and most preferably 40 to 70% by weight of carbon and hydrogen-containing compounds, based on the total weight of the particulate carbon-containing raw material.

[0081] The particulate carbon-containing raw material may contain inert compounds, which may include metals, metallic compounds, silicon, and silica. The metals may be zinc, sulfur, silicon, calcium, aluminum, and / or iron.

[0082] The particulate carbon-containing raw material may contain 1 to 40% by weight of an inert compound, preferably 3 to 30% by weight of an inert compound, more preferably 4 to 20% by weight of an inert compound, and most preferably 5 to 15% by weight of an inert compound, based on the total weight of the particulate carbon-containing raw material.

[0083] The particulate carbon-containing material may further contain carbon black, i.e., recovered carbon black. Carbon black is typically present in tires and can therefore be recovered. The particulate carbon-containing material should contain 1 to 70% by weight of carbon black, preferably 5 to 60% by weight, more preferably 10 to 50% by weight, and most preferably 15 to 40% by weight, based on the total weight of the particulate carbon-containing material. Alternatively, the particulate carbon-containing material may not contain recovered carbon black.

[0084] In this context, recovered carbon black in this method means recoverable carbon black. In other words, it is carbon black that is present in the raw materials and not produced by the method of the present invention.

[0085] C,H-containing compounds are, for example, rubber, plastics, and / or biomass-based materials. The particulate carbon-containing raw material is preferably provided in granule form. Therefore, the particulate carbon-containing raw material may include rubber granules, plastic granules, and / or biomass-based granules. Thus, the particulate carbon-containing raw material can be particulate rubber raw material, particulate plastic raw material, and / or particulate biomass-based raw material. The particulate carbon-containing raw material preferably includes rubber granules, and the rubber granules preferably contain carbon black.

[0086] Biomass-based raw materials have a C14 content ( 14 By measuring the C content (radiocarbon dating), it is possible to distinguish it from fossil raw materials. The relative amount of C14 atoms compared to C12 (C14 to C12 ratio / 14 C / 12The carbon-to-carbon ratio is lower in fossil fuels compared to biomass fuels. Therefore, fossil fuels have a lower relative amount of C14 atoms compared to C12 than their relative amount in naturally occurring sources.

[0087] Preferably, the amount of particulate biomass-based raw material in the particulate carbon-containing raw material is 20-100% by weight, for example, 40-100%, 50-99%, 60-95%, or 80-90% by weight, based on the total weight of the particulate carbon-containing raw material.

[0088] Preferably, the amount of rubber granules in the particulate carbon-containing raw material is 20 to 100% by weight, for example, 40 to 100% by weight, 50 to 99% by weight, 60 to 95% by weight, or 80 to 90% by weight, based on the total weight of the particulate carbon-containing raw material.

[0089] Preferably, the amount of particulate plastic raw material in the particulate carbon-containing raw material is 20 to 100% by weight, for example, 40 to 100% by weight, 50 to 99% by weight, 60 to 95% by weight, or 80 to 90% by weight, based on the total weight of the particulate carbon-containing raw material.

[0090] Particulate biomass-based carbon black raw materials may include plant-based raw materials, preferably non-edible plant-based raw materials and / or waste plant-based raw materials. As used herein, the term “non-edible” refers to materials that are not suitable for human consumption. The term “waste” refers to materials that are discarded or disposed of, for example, after use, as unsuitable or no longer useful for the intended purpose.

[0091] Particulate biomass-based carbon black raw materials may include wood, grass, cellulose, hemicellulose, lignin, and / or natural rubber.

[0092] As used herein, the term “wood” refers to the porous and fibrous structural tissue found in the stems and roots of trees and other woody plants. Suitable examples of wood include, but are not limited to, pine, spruce, larch, juniper, ash, hornbeam, birch, alder, beech, oak, pin, horse chestnut, mulberry, or mixtures thereof. Suitable examples of grass include, but are not limited to, cereal grasses such as maize, wheat, rice, barley, or millet; bamboo and grass in natural grasslands, as well as species cultivated in lawns and pastures. Suitable examples of lignin include, but are not limited to, lignin and lignosulfonates removed by the Kraft process.

[0093] Rubber granules may include natural rubber and / or synthetic rubber. Particulate carbon-containing raw materials may include rubber granules containing carbon black. Natural rubber may be derived from rubber trees (Helvea brasiliensis), guayule, and dandelion. Rubber granules may be used in tires, cable sheaths, tubes, conveyor belts, shoe soles, hoses, or mixtures thereof.

[0094] Examples of synthetic rubbers include styrene-butadiene rubber such as emulsion-styrene-butadiene rubber (ESBR) and solution-styrene-butadiene rubber (SSBR), polybutadiene, polyisoprene, ethylene-propylene-diene rubber (EPDM), ethylene-propylene rubber (EPM), butyl rubber, halogenated butyl rubber, chlorinated polyethylene, chlorosulfonated polyethylene, acrylonitrile-butadiene rubber, hydrogenated acrylonitrile-butadiene rubber, polychloroprene, acrylate rubber, ethylene-vinyl acetate rubber, ethylene-acrylic rubber, epichlorohydrin rubber, silicone rubber, fluorosilicone rubber, fluorocarbon rubber, or mixtures or combinations thereof.

[0095] The plastic granules or particulate plastic raw materials can be any plastic known in the art. For example, acrylics such as poly(acrylic acid) or poly(methyl methacrylate), polyesters such as polyethylene terephthalate or polyethylene glycol, polyurethanes such as those derived from toluene diisocyanate (TDI) or methylenediphenyl diisocyanate, polyolefins such as polypropene or polyethylene, or polystyrene. Generally, thermoplastics and thermosetting materials can be used.

[0096] The plastic granules are preferably derived from household waste materials, such as plastic bags, plastic containers, and plastic packaging.

[0097] The raw material is preferably provided in granular form. This can be achieved by grinding to a desired particle size or granular size. For example, tires can be ground to obtain rubber granules as a raw material.

[0098] The particulate carbon-containing raw material, comprising at least 50% by weight, preferably at least 60% by weight, more preferably at least 70% by weight, and most preferably at least 80% by weight, is preferably having a particle size of 125 μm to 2 mm, preferably 125 μm to 1 mm, more preferably 250 μm to 1 mm, and most preferably 500 μm to 1000 μm, and this particle size is measured according to ASTM D1511-12 (2017).

[0099] The particulate carbon-containing raw material, comprising at least 70% by weight, preferably at least 80% by weight, more preferably at least 90% by weight, and most preferably at least 98% by weight, is preferably having a particle size of less than 2 mm, preferably less than 1 mm, more preferably less than 500 μm, and most preferably less than 250 μm, which is measured according to ASTM D1511-12 (2017).

[0100] The particulate carbon-containing raw material, comprising at least 70% by weight, preferably at least 80% by weight, more preferably at least 90% by weight, and most preferably at least 98% by weight, is preferably having a particle size of less than 500 μm, which is measured according to ASTM D1511-12 (2017).

[0101] The particulate carbon-containing raw material, comprising at least 70% by weight, preferably at least 80% by weight, more preferably at least 90% by weight, and most preferably at least 98% by weight, is preferably having a particle size of less than 1 mm, which is measured according to ASTM D1511-12 (2017).

[0102] The particulate carbon-containing raw material, comprising at least 70% by weight, preferably at least 80% by weight, more preferably at least 90% by weight, and most preferably at least 98% by weight, is preferably having a particle size of less than 2 mm, preferably less than 250 μm, and this particle size is measured according to ASTM D1511-12 (2017).

[0103] The particulate carbon-containing raw material, which contains less than 1% by weight, preferably at least 0.5% by weight, more preferably less than 0.1% by weight, and most preferably less than 0.01% by weight, is desirable to have a particle size greater than 2 mm, preferably greater than 1 mm, more preferably greater than 500 μm, and most preferably greater than 250 μm, and this particle size is measured according to ASTM D1511-12 (2017).

[0104] The particulate carbon-containing raw material is particularly preferably having a particle size of less than 2 mm, preferably less than 1 mm, more preferably less than 500 μm, and most preferably less than 250 μm, and this particle size is measured according to ASTM D1511-12 (2017).

[0105] The particle size of the raw material can be controlled by classifying the particulate carbon-containing raw material before it is injected into the reactor. Therefore, it is preferable that the particulate carbon-containing raw material be classified before it is injected into the reactor or into the mixing and feeding unit.

[0106] Classification can be carried out by any means known in the art, such as sieving or other classification methods. Classification can be carried out using vibrating screens, rotating screens, cyclones, elutriation classifiers, air jet screens and / or dynamic air classifiers. Any combination of the foregoing can be used. Classification can be used to obtain the maximum or minimum desired particle size as described herein.

[0107] The particle size of the raw material can be controlled by sieving the particulate carbon-containing raw material before injecting it into the reactor. Sieve sizes such as those described in ASTM D1511-12 (2017) can be used. For example, sieves with openings of 2000 μm, 1000 μm, 500 μm, 250 μm, or 125 μm, preferably 500 μm, 250 μm, or 125 μm, can be used. Furthermore, the openings of the sieve can be sized to capture particles larger than 2000 μm, larger than 1000 μm, larger than 500 μm, larger than 250 μm, or larger than 125 μm, preferably larger than 500 μm, larger than 250 μm, or larger than 125 μm.

[0108] The particulate carbon-containing raw material, which is 10% by weight or less, preferably 5% by weight or less, more preferably 4% by weight or less, and most preferably 2% by weight or less, should have a particle size greater than 4 mm, preferably greater than 2 mm, more preferably greater than 1 mm, and most preferably greater than 0.5 mm, and this particle size is measured according to ASTM D1511-12 (2017).

[0109] The particulate carbon-containing raw material, which is 10% by weight or less, preferably 5% by weight or less, more preferably 4% by weight or less, and most preferably 2% by weight or less, should have a particle size of less than 150 μm, preferably less than 125 μm, more preferably less than 110 μm, and most preferably less than 100 μm, and this particle size is measured according to ASTM D1511-12 (2017).

[0110] None of the particles of the particulate carbon-containing raw material should have a particle size of 1 mm or larger, preferably 500 μm or larger, more preferably 250 μm or larger, and most preferably 125 μm or larger, and this particle size should be measured according to ASTM D1511-12 (2017).

[0111] The particle size distribution of the particulate carbon-containing raw material can be measured according to ASTM D1511-12(2017), where (a) sieve number 10 holds 1 to 10% by weight, preferably 1 to 8% by weight, more preferably 1 to 5% by weight, most preferably 1 to 3% by weight of the particulate carbon-containing raw material, and / or (b) sieve number 18 holds 1 to 25% by weight, preferably 2 to 20% by weight, more preferably 4 to 15% by weight, most preferably 5 to 12% by weight of the particulate carbon-containing raw material, and / or (c) sieve number 35 holds 10 to 80% by weight, preferably 15 to 70% by weight, more preferably 20 to 60% by weight, most preferably 25 to 55% by weight of the particulate carbon-containing raw material. (d) Sieve No. 60 holds particulate carbon-containing raw material in amounts of 5-70% by weight, preferably 10-60% by weight, more preferably 15-50% by weight, most preferably 20-45% by weight, and / or (e) Sieve No. 120 holds particulate carbon-containing raw material in amounts of 1-80% by weight, preferably 7-70% by weight, more preferably 5-60% by weight, most preferably 7-50% by weight, and / or (f) the bottom tray contains particulate carbon-containing raw material in amounts of less than 4% by weight, preferably less than 3% by weight, more preferably 0-2% by weight, most preferably 0.01-1% by weight. It is desirable to independently select the desired range for each sieve.

[0112] The 50% by weight cumulative particle size of the particulate carbon-containing raw material should be 100 μm to 4 mm, preferably 100 μm to 3 mm, more preferably 100 μm to 2 mm, and most preferably 100 μm to 500 μm, where the 50% by weight cumulative particle size is measured according to ASTM D1511-12 (2017). The 50% by weight cumulative particle size can be interpolated using standard techniques known in the art. It is particularly preferable to interpolate the 50% by weight cumulative particle size using the Rosin-Rammler-Sperling-Bennett distribution (RRSB distribution).

[0113] The weight-average particle size Dw50 of the particulate carbon-containing raw material may be 100 μm to 4 mm, preferably 100 μm to 3 mm, more preferably 100 μm to 2 mm, and most preferably 100 μm to 500 μm, and the weight-average particle size Dw50 is measured according to ASTM D1511-12 (2017).

[0114] The particle size distribution Dw10 of the particulate carbon-containing raw material may be 100 μm to 250 μm, preferably 110 μm to 220 μm, more preferably 120 μm to 210 μm, and most preferably 130 μm to 200 μm, and this particle size distribution Dw10 is measured according to ASTM D1511-12 (2017).

[0115] The particle size distribution Dw90 of the particulate carbon-containing raw material may be 400 μm to 4 mm, preferably 500 μm to 3 mm, more preferably 600 μm to 2 mm, and most preferably 700 μm to 500 μm, and this particle size distribution Dw90 is measured according to ASTM D1511-12 (2017).

[0116] The particle size distribution range of the particulate carbon-containing raw material (Dw90-Dw10) / Dw50 may be 0.4 to 2.5, preferably 0.7 to 2, more preferably 1 to 1.8, and most preferably 1.2 to 1.7, where the particle size distributions Dw10, Dw50, and Dw90 are measured according to ASTM D1511-12 (2017).

[0117] Dw50, Dw10, and Dw90 can be interpolated using standard techniques known in the art. Interpolating Dw50, Dw10, and Dw90 using the Rosin-Rammler-Sperling-Bennett distribution (RRSB distribution) is particularly preferred.

[0118] The particle size, or granule size, is affected by the heating rate of the raw materials in the reactor. Smaller granules or particles have a higher specific surface area, allowing for a higher heating rate. A fast heating rate is beneficial because it allows the particulate raw materials to evaporate and then thermally decompose. Thermal decomposition is considered to be significantly faster than the evaporation of the particulate raw materials. The heating rate can also be increased by increasing the temperature of the high-temperature gas flow.

[0119] Carbon black (including rCB) and / or particulate carbon-containing raw materials manufactured as described above are subject to ASTM By measuring according to Method B (AMS) of D6866-20, it is possible to have a pMC (modern carbon content) of 1% or more, for example, 2% or more, 5% or more, 7% or more, 10% or more, 12% or more, 15% or more, 17% or more, 20% or more, 22% or more, 25% or more, 27% or more, 30% or more, 32% or more, 35% or more, 37% or more, 40% or more, 42% or more, 45% or more, 47% or more, 50% or more, 52% or more, 55% or more, 57% or more, 60% or more, 62% or more, 65% or more, 67% or more, 70% or more, 72% or more, 75% or more, 77% or more, 80% or more, 82% or more, 85% or more, 87% or more, 90% or more, 92% or more, 95% or more, 97% or more, or 99% or more. For each sample, 14 C / 13 The ratio of C is calculated and compared with the measurement value obtained using the oxalic acid II standard (NIST-4990C). The measured value (pMC) is corrected by d13C measured using an isotope ratio mass spectrometer (IRMS). Carbon black can have a pMC (modern carbon content) of preferably 10% or more, particularly preferably 15% or more, more preferably 50% or more, even more preferably 85% or more, and most preferably 90% or more, as measured according to ASTM D6866-20 Method B (AMS). Carbon black can have a pMC (modern carbon content) of 100% as measured according to ASTM D6866-20 Method B (AMS).

[0120] The resulting carbon black typically includes recovered carbon black and new carbon black. Recovered carbon black is generally obtained when the particulate carbon-containing raw material contains carbon black. New carbon black is obtained by thermal decomposition, i.e., by the method described above.

[0121] The mass flow rate of the raw materials should be adjusted so that the raw materials are heated uniformly. The particulate carbon-containing raw materials should be injected into the reactor at a mass flow rate of 2 to 50 kg / h per 130 L of reactor reaction volume, preferably 5 to 40 kg / h per 130 L of reactor reaction volume, more preferably 8 to 30 kg / h per 130 L of reactor reaction volume, and most preferably 10 to 20 kg / h per 130 L of reactor reaction volume.

[0122] The fuel may include gaseous or liquid hydrocarbons, preferably natural gas, fuel oil, or H2.

[0123] Hydrogen can be used as a carrier gas and / or fuel for carbon black production. Hydrogen is preferably used as a carrier gas and fuel for carbon black production. Hydrogen is used as a carrier gas when it is present in a molar excess relative to oxygen in the combustion mixture. Therefore, hydrogen should be present in the high-temperature combustion gas and high-temperature reaction mixture.

[0124] The high-temperature gas flow should have a temperature of 900 to 3500°C, preferably 950 to 3000°C, more preferably 1000 to 2000°C, and most preferably 1200 to 1900°C.

[0125] High-temperature gas flows can be obtained by electric preheating, plasma, and combustion of fuel and oxygen-containing gases. Combustion of fuel and oxygen-containing gases is preferably carried out in a furnace reactor. However, as mentioned above, other means of providing the desired temperature of the high-temperature gas flow are also conceivable.

[0126] The reactor can be a co-flow reactor. A co-flow reactor can be a furnace reactor. A furnace reactor can have a flow path along the central longitudinal axis of the reactor. The reactor includes, in the following order from upstream to downstream (flow direction): a combustion chamber, a choke, and a tunnel equipped with quenching means. These components define a flow path along the central longitudinal axis of the reactor for a high-temperature gas flow, such as a high-temperature combustion gas. Therefore, the components should be fluidly connected, in particular, along the central longitudinal axis of the reactor.

[0127] A tubular conduit can be connected to the combustion chamber to supply the oxygen-containing gas necessary for the combustion of the fuel (or combustion fuel). The tubular conduit may also be positioned along the central longitudinal axis of the reactor so that the replenishment of oxygen-containing gas occurs along the aforementioned flow path. Furthermore, the reactor may include fuel injection means for injecting fuel into the combustion chamber.

[0128] Generally, fuel lances are used to supply fuel to the combustion chamber. The combustion chamber can be connected to a tubular conduit running from downstream to upstream to allow oxygen-containing gas to be supplied to the combustion chamber. The combustion chamber is positioned along the central longitudinal axis of the reactor.

[0129] The combustion chamber is preferably formed from an internal refractory lining covered by a gas stopper, such as a metal cover. The material forming the refractory and the outer lining may be 70% alumina (Al2O3) and may be a castable refractory such as Kaocrete® 32cm, which has a melting point of about 1870°C and is conventionally found in the art. Furthermore, one can rely on brick refractories such as RUBY SR (Harrison-Walker Refractories, Pittsburgh, Pennsylvania), which consists of 84.5% alumina with 9.8% chromium oxide (Cr2O3) and has a melting point of about 2050°C. The shell or lining is preferably formed from carbon steel, except for any piping that comes into contact with high-temperature process air. In such areas, the piping is formed from "316 stainless steel".

[0130] The combustion chamber is preferably sized as a cylinder. A constriction (choke) may be provided downstream of the combustion chamber. The constriction has a tapered passage that converges from upstream to downstream. Preferably, these constrictions have a truncated cone-shaped passage. The combustion chamber may also have a taper from downstream to upstream. Thus, the combustion chamber may include a region that tapers toward the reaction chamber and / or toward a tubular conduit.

[0131] Typically, the oxygen-containing gas is preheated to a temperature of 200-1600°C, preferably 350-1400°C, more preferably 500-1200°C, and most preferably 450-950°C.

[0132] Typically, the fuel is preheated to a temperature of 50-750°C, preferably 100-700°C, more preferably 300-700°C, and most preferably 450-650°C.

[0133] Preheating of oxygen-containing gases and fuels can be done electrically or using heat exchangers. Preheating hydrogen and / or oxygen-containing gases is particularly preferred because, for example, less energy needs to be generated from the combustion of the fuel.

[0134] Furthermore, another advantage is the reduced preheating and oxygen-containing gas requirements, as the high-temperature combustion mixture and high-temperature reaction mixture contain very little water (H2O). Water affects the surface properties of the resulting carbon black.

[0135] The tunnel is generally connected to the combustion chamber so that the high-temperature combustion gases obtained in the combustion chamber can flow into the tunnel. The tunnel can be positioned along the central longitudinal axis of the reactor. The diameter of the reaction chamber can be larger than the diameter of the constricted section of the combustion chamber so that the high-temperature combustion gases can expand. The expansion section is preferably sized as a cylinder and communicates with the combustion chamber, preferably with the constricted section (choke) of the combustion chamber.

[0136] Particulate carbon-containing material can be injected into the combustion chamber, the choke, and / or the tunnel of the furnace reactor. Typically, particulate carbon-containing material is injected into the choke (constriction).

[0137] When particulate carbon-containing raw materials are injected, for example, into a combustion chamber, the particulate carbon-containing raw materials or the carrier gas containing them should have a desirable pressure. This means that the pressure of the particulate carbon-containing raw materials or the carrier gas containing them must be higher than the pressure inside the combustion chamber. Therefore, a suitable feed-mixing device configured to operate under pressurized conditions should be used.

[0138] The particulate carbon-containing raw material should be injected through multiple inlets, preferably radially and perpendicularly to the central longitudinal axis of the reactor.

[0139] The concentration of O2 in the high-temperature gas stream is less than 5% by volume, preferably less than 4% by volume, more preferably 0.01 to 3% by volume, and most preferably 0.1 to 2% by volume.

[0140] The particulate carbon-containing raw material may be injected into the reactor via a raw material injection means. The raw material injection means may include a plurality of injection nozzles or lances, preferably arranged circumferentially with respect to the central longitudinal axis. This circumferential arrangement allows for homogeneous mixing of the carbon black raw material with the high-temperature combustion gas, further improving the uniformity of the carbon black. The particulate carbon-containing raw material can be introduced through a plurality of raw material injection means.

[0141] For example, this can be carried out using a raw material lance pipe extending in the axial direction and a radially extending raw material injector having a nozzle capable of generating various conical sprays (e.g., conical spray angles of 15, 30, 45, and 60 degrees).

[0142] To produce the desired carbon black characteristics, radially extending raw material injectors may be equipped with shut-off valves so that the raw material is introduced only through a specific raw material injector, or so that the flow rate of the raw material flowing through the injector changes.

[0143] The raw material injection means is preferably connected to a feed mixer. It is desirable that one feed mixer supplies multiple raw material inlets. However, it is also possible to use two or more feed mixers.

[0144] The tunnel is a means for injecting a rapid coolant into a flow path along the central longitudinal axis of the reactor and may include means located behind the flow direction for injecting the raw materials for carbon black. Alternatively, the rapid cooling means may be a rapid boiler or a heat exchanger.

[0145] The tunnel may include means for injecting a rapid coolant into a flow channel along the central longitudinal axis of the reactor. The means for injecting the rapid coolant are positioned in the direction of flow following the means for injecting the raw materials for carbon black. The rapid coolant is generally H2O.

[0146] The distance between the raw material injection means and the means for injecting the rapid refrigerant (first means for injecting the rapid refrigerant) can be 150 to 80,000 mm, preferably 900 to 50,000 mm, more preferably 1,500 to 30,000 mm, and most preferably 2,500 to 20,000 mm.

[0147] The means for injecting the rapid coolant can extend into the tunnel. For example, a cooling fluid conduit or multiple radial cooling fluid conduits can be used. The rapid coolant, such as a cooling fluid (e.g., water), is sprayed into the tunnel to stop the carbon black reaction at the appropriate time and place.

[0148] The reactor may further include tubular conduits for supplying oxygen-containing gas to the combustion chamber. The oxygen-containing gas (O2-containing gas or O2-containing gas mixture) may be air, oxygen-enriched air, other oxygen-containing gases, and / or pure oxygen. In this way, the tubular conduits can be connected to the combustion chamber, thereby allowing the oxygen-containing gas to flow through the tubular conduits within the combustion chamber. The tubular conduits may be positioned along the central longitudinal axis of the reactor. It is desirable that the central longitudinal axis of the tubular conduits be coaxial with the central longitudinal axis of the reactor. Thus, the tubular conduits can be positioned coaxially along the central longitudinal axis of the reactor. The weight percentage of oxygen present in the oxygen-containing gas should be 20-100% by weight, preferably 50-99% by weight, more preferably 60-95% by weight, and most preferably 70-90% by weight, where the weight percentage is based on the total weight of the oxygen-containing gas.

[0149] The tubular conduit can have a cylindrical shape that extends along the central longitudinal axis of the reactor without curving.

[0150] The inner diameter of the tubular conduit for supplying oxygen-containing gas can be 5 cm to 3 m, for example, 10 cm to 3 m, 20 cm to 3 m, 9 cm to 2.5 m, 13 cm to 1.5 m, 0.1 m to 2 m, 20 cm to 1 m, 30 cm to 1.5 m, 15 cm to 60 cm, or 15 cm to 90 cm.

[0151] The inner diameter is preferably constant over the entire tubular conduit, but the tubular conduit may also have two different sections connected to an inlet funnel in which the inner diameter of the tubular conduit decreases in the flow direction (i.e., the direction of the combustion chamber). Thus, the tubular conduit may have a first section having a first inner diameter and a second section having a second inner diameter smaller than the first inner diameter. The first inner diameter can be in the range of 5cm to 3m, for example, 20cm to 3m, 9cm to 2.5m, 13cm to 1.5m, 0.1m to 2m, 20cm to 1m, 30cm to 1.5m, 15cm to 60cm, or 15cm to 90cm, and the second inner diameter can be in the range of 5cm to 3m, for example, 20cm to 3m, 9cm to 2.5m, 13cm to 1.5m, 0.1m to 2m, 20cm to 1m, 30cm to 1.5m, 15cm to 60cm, or 15cm to 90cm.

[0152] A fuel injection means for introducing any suitable combustion fuel (e.g., natural gas, fuel oil, or other gaseous or liquid hydrocarbons, preferably natural gas or fuel oil, or H2) can be configured in various ways. For example, the injection means may be located at the end of a tubular conduit, which is connected to a combustion chamber. For example, the injection means may be a tubular injection pipe positioned circumferentially with respect to the central longitudinal axis of the tubular conduit, so that the angle of incidence of the fuel is substantially perpendicular to the flow direction of the oxygen-containing gas.

[0153] However, in addition to the fuel lance, multiple fuel injection means can also be provided. For example, at the end of the tubular conduit, additional fuel injection means can be arranged rotationally symmetrically with respect to the central longitudinal axis of the tubular conduit.

[0154] The oxygen-containing gas is generally supplied in an amount that results in an excess of oxygen relative to the amount of oxygen for complete combustion of the fuel, and / or the oxygen-containing gas is supplied in an amount where the k value is in the range of 0.01 to 10, preferably 0.1 to 5, more preferably 0.5 to 2, and most preferably 0.7 to 1. Here, the k value is defined by the ratio of the stoichiometric amount of O2 required for complete stoichiometric combustion of the fuel to the amount of O2 supplied.

[0155] The flow rates of the fuel and the oxygen-containing gas can be adjusted to be at a high temperature and are usually kept at values close to the stoichiometric ratio. The ratio has to be adjusted to prevent melting of the refractory. The range of the oxygen-containing stream is very wide, for example, from a low of about 1000 Nm 3 / h to a high of about 100 kNm 3 / h, e.g., 1000 Nm 3 / h to 100 kNm 3 / h, 1000 Nm 3 / h to 10 kNm 3 / h, 2000 Nm 3 / h to 3000 Nm 3 / h, or 1000 Nm 3 / h to 2000 Nm 3 / h. However, the present invention is not limited to these amounts, and in larger reactors, more air flow is required, while in smaller reactors, less air flow is required.

[0156] The desired temperature of the high-temperature gas stream can also be achieved by plasma heating the gas stream. The gas stream can be preheated as described above.

[0157] A plasma torch can provide the plasma for the heating described above. A design for a plasma torch is described in WO1993 / 012633A1. However, any means known in the art for generating plasma can be used. The plasma can be formed by a plasma carrier gas heated by an electric arc burning between electrodes. Plasma processing is possible in a high-temperature plasma zone from 3000°C to 20,000°C. The plasma carrier gas can be oxygen or hydrogen. Hydrogen is particularly preferred as the plasma carrier gas.

[0158] Microwave plasma can also provide the plasma for the aforementioned processing. For example, a microwave generator can be used to provide microwave radiation within the reaction chamber. Microwave radiation having a frequency of 1 to 300 GHz can be used. Alternatively, the plasma can be generated using a high-frequency power supply (RF generator).

[0159] The residence time between the injection time of the particulate carbon-containing raw material into the reactor and the quenching time of the resulting mixture should be 150 ms to 4 seconds, preferably 200 ms to 3 seconds, more preferably 250 ms to 2 seconds, and most preferably 250 ms to 1 second. The residence time of the particulate carbon-containing raw material means the time it takes for the particulate carbon-containing raw material to evaporate and be thermally decomposed. The quenching of the resulting mixture stops the thermal decomposition of the particulate carbon-containing raw material. The heating rate of the particulate carbon-containing raw material is lower compared to the liquid raw material, and therefore, the evaporation and thermal decomposition of the particulate carbon-containing raw material generally require more time.

[0160] The residence time of the particulate carbon-containing raw material should be 150 ms to 4 seconds, preferably 200 ms to 3 seconds, more preferably 250 ms to 2 seconds, and most preferably 250 ms to 1 second, where the residence time is calculated according to formula (1).

number

[0161] The volumetric flow rate is the volume of fluid per unit second after the injection of particulate carbon-containing raw material into a high-temperature gas stream, and preferably, the volume of the fluid is calculated according to the ideal gas law according to equation (2).

number

[0162] The reaction volume of the reactor is the volume of the reactor between the injection point of the particulate carbon-containing raw material and the quenching point.

[0163] The residence time should be selected so that the C and H-containing materials in the particulate carbon-containing raw material are completely thermally decomposed.

[0164] The absolute temperature for calculating the volumetric flow rate can be measured directly within the reactor. In particular, the temperature is measured immediately after the injection of the raw materials into the reactor, for example, 50 mm behind the injection. For example, the temperature can be measured with a pyrometer.

[0165] Alternatively, the absolute temperature T (for calculating volumetric flow rate) can be calculated as follows. The above calculation considers the combustion of fuel in a furnace reactor. This method includes the combustion of fuel and the heating of rubber granules to the reaction temperature. Residual oxygen from combustion does not result in complete combustion. Therefore, it is inferred that CO and H2O with the same CO / H2O ratio are formed according to the C / H ratio of the raw materials.

[0166] The reaction temperature can be calculated from the energy balance.

number

[0167] The mass flow rate of the fuel is m F It is represented by h F m is the difference in thermal enthalpy between the temperature and pressure at the fuel inlet to the combustor and the fuel under standard conditions (T=25°C, P=101325Pa). A is the mass flow rate of the inert species, h A ΔH is the difference in the thermal specific enthalpy of inert species A between the conditions (TA,PA) of 25°C and 1.01325 bar and the inert species introduced into the combustor. The number of inert substances is denoted by K. Inert species are those that do not change in an ideal process. These inert substances include, for example, nitrogen, carbon black, minerals, and water. uF This is the lower heating value of the fuel at a temperature of 25°C and a pressure of P=101325Pa. The difference in the thermal enthalpy of oxygen between the supply conditions and the reference conditions (T=298.15K, P=101325Pa) is h. O2 This is shown, and the oxygen mass flow rate is m O2This is shown as follows: The difference in the specific thermal enthalpy of the reaction product i between the conditions of reaction temperature T and P=101325Pa and the reference conditions (T=298.15K, P=101325Pa) is h i It is represented as follows. The corresponding mass flow meter is mp i The lower heating value of this compound is shown as H ui This is shown. When particulate raw materials are transported into the reactor along with the gas flow, the gas mass flow rate is m T The difference in thermal enthalpy between the conditions at the reactor inlet for this mass flow rate and the reference conditions (T=25°C, P=103125Pa) is given by h T As shown by H uT is the corresponding lower specific heat output. Heat loss is Q Loss This is taken into consideration. The mass flow rate of the hydrocarbon portion of the particulate raw material is m R It can be expressed as follows and calculated using the following formula.

number

[0168] The lower heating value is measured according to DIN 5499 and DIN 51857. If the gas is not reported in DIN 51857, the heating value can be determined by the heat of formation. These values ​​are available in "The Properties of Gases and Liquids," NIST Data Book, etc. Chemical species C x H y S z O w And, based on the assumption of total oxidation of gaseous water as a reaction product, the following equation is obtained.

number

[0169] A is an unoxidized substance. f p = fe. The amount of heat generated is given by the following formula.

number

[0170] If the reference temperature for the heat of formation differs from that of substance i (298.15 K), the amount of heat can be calculated using the molar heat capacity.

number

[0171] Molar heat capacity can be found using the same textbook, such as "Properties of Gases and Liquids" or the NIST Data Book.

[0172] When the fuel consists of more than one type, the lower heating value can be determined by the following formula.

number

[0173] The mass fraction of component I is ξ i This is shown, and the lower heating value of component i is ΔH u,i This is shown by and the number of species in the fuel is shown by P.

[0174] The difference in thermal enthalpy of fuels containing more than one type of fuel is calculated using the following formula.

number

[0175] The average molecular weight of the fuel is determined by the following formula.

number

[0176] If the composition is unknown, the lower heating value is measured by a calorimeter. If the fuel is solid or liquid, the lower heating value is measured according to DIN 51900. From the experimental results, the water content was measured according to ASTM D4928-12 (2018), and the sulfur and hydrogen content were measured according to the methods described in the examples.

[0177] The difference in thermal enthalpy of the exhaust gas between T=298.15K and the flame temperature can be obtained by the following formula.

number

[0178] The number of species in the generated gas stream is denoted by N, and the average molecular weight of the exhaust gas is M. Gas This is shown, and this average molecular weight is determined by the following formula.

number

[0179] The lower heat of release of inert species in the product stream is set to 0 J / mol.

[0180] To determine the lower heating value of hydrocarbon species in particulate matter, it is necessary to determine the micro-Conradson content according to the water content (ASTM D4928-12(2018)) and ASTM D4530-15(2020). Furthermore, the final analysis of particulate matter must be measured according to ASTM D3176-15(2016), and the total heating value must be measured according to ASTM D4809:2018.

[0181] The lower heating value of particulate raw materials is calculated using the following formula.

number

[0182] Furthermore, the lower heating value of the Conradson residue can be determined by measuring the total calorific value and hydrogen content of the Conradson residue using the same equation. The water content of Conradson is 0. The lower heating value of hydrocarbon-containing particulate raw materials is determined by the following formula.

number

[0183] The C / H ratio of the hydrocarbon portion can be determined from the final analysis of the particulate raw material and the final analysis using Conradson.

number

[0184] The molar enthalpy difference of water can be determined by the following formula.

number

[0185] In the case of CO2, it can be obtained by the following formula.

number

[0186] In the case of SO2

number

[0187] In the case of N2

number

[0188] In the case of O2

number

[0189] In the case of CO

number

[0190] The lower heating value of CO is H u,CO = 282980 J / mol.

[0191] In the case of gaseous rubber products

number

[0192] In the case of particulate rubber, it can be obtained by the following formula.

number

[0193] In Conradson's case

number

[0194] Calculation example

[0195] Combustion of methane entering the combustion chamber at a temperature of 3 bar and T=290K.

[0196] The standard volumetric flow rate of methane is 13 Nm³, considering a pressure of 101325 Pa and a temperature of T = 273.15 K. 3 Assuming the rate is / h(STP), the standard volumetric flow rate of nitrogen at temperature T=673.15K and pressure 1.2bar is calculated as 118.5Nm³, taking into account pressure 101325Pa and temperature T=273.15K. 3 Assuming the oxygen flow rate is / h(STP), and considering the standard temperature T=273.15K and standard pressure P=101325Pa, the standard oxygen flow rate is 31.5Nm³. 3 Let's use / h(STP).

[0197] Inside the chalk, rubber granules are supplied to a system with a mass flow rate of 20 kg / h, at a temperature of 20°C and a pressure of 1 bar.

[0198] The lower heating value of methane is 802.6 MJ / kmol at T=298.15K and P=101325Pa, according to DIN51857. The heat capacity of methane can be obtained from "Properties of Gases and Liquids," and its value is as follows: Cp(T)=8.314462*(4.568-8.975 / 10^3*T+3,631 / 10^5*T^2-3.407 / 10^8*T^3+1.091 / 10^11*T^4) Formula (22)

[0199] Therefore, we obtain h_f by the following equation.

number

[0200] The temperature of the fuel supply is symbolized by T, given by T=290K in this example, and the reference temperature for calorific value is given by T0=298.15K.

[0201] The enthalpy difference between T=298.15K and the supply temperature can be determined, and for inert gas nitrogen, it can be determined by equation (4). The enthalpy difference for oxygen can be determined by equation (15).

[0202] Heat loss occurs on the reactor shell, and heat transfer can be calculated according to the VDI thermal atlas based on the measured temperature of the shell. Heat transfer should be considered in terms of radiation and convection / free convection.

[0203] Calculation of the mass flow rate of the compound in the reaction region

[0204] In equation (4), let x=1, y=4 and z=0, w=0, p=0. Therefore, 13Nm of methane 3 / h, 13Nm of CO2 3 / h, and 26Nm of water 3 / h is obtained. The remaining oxygen is determined by subtracting the oxygen flow rates in the form of CO2 and H2O (SO2 if sulfur is present in the fuel) from the total oxygen flow rate. The conversion between mass flow rate and standard volume flow rate for a gas species is performed by the following formula.

number

[0205] Therefore, the remaining oxygen flow rate is obtained.

number

[0206] The remaining oxygen is estimated to be converted by the hydrogen and carbon in the granular rubber portion, according to the atomic H / C ratio of the rubber portion. If the H / C ratio is 2, one H2O and one CO are obtained. Therefore, the water flow already calculated is 5.5 Nm of H2O. 3 Adding the flow rate of / h, the total is 31.5 Nm 3 H2O at / h and 5.5Nm 3 Obtain CO at 8 Nm. The rubber granules are 8 Nm 3 It is transported to the reactor with nitrogen at a rate of / h.

[0207] These gas flows are converted to mass flow rates using the above equation, leading to the following: N2158.02 kg / h CO2 25.519 kg / h H2O 20.88 kg / h CO 6.87 kg / h H2O added: 4.42 kg / h

[0208] The rubber mass flow rate in the gas phase is calculated by subtracting the inert species from the total rubber granule flow rate, and then subtracting the mass flow rate of burned rubber.

number

[0209] Conradson is treated as an inert material calculated as follows.

Number

[0210] Calculation of heat loss

[0211] The heat flux can be calculated by the following formula.

Number

[0212] In the case of free convection α, it is calculated as a function of the Rayleigh number and the Prandtl number Pr by the Nusselt number.

Number

[0213] Using the following formula,

Number

[0214] The Rayleigh number is calculated by the following formula.

Number

[0215] Integrating all of these into the energy balance gives the following formula.

Number

[0216] The reactor has an outer surface area of 15.9 m 2 and thus is at 1629 °C in this example. The reaction volume is 0.162 m 3 The volumetric flow rate of all species except micro Conradson is 1236 m 3It is / h. Therefore, the residence time is obtained by the following equation,

number

[0217] Generally, the residence time is selected so that the C and H-containing materials in the particulate carbon-containing raw material are completely thermally decomposed.

[0218] The formation of carbon black is generally completed by rapid cooling of a high-temperature gas stream. Therefore, a method for producing carbon black may further include the step of rapidly cooling a high-temperature gas stream after injection in step (d).

[0219] The transmittance can serve as an indicator of whether the residence time is sufficient for the complete thermal decomposition of the raw materials, for example, C and H-containing materials. Therefore, (e) the high-temperature gas stream should be quenched such that the transmittance of the obtained carbon black at 425 nm is at least 20%, preferably at least 30%, more preferably at least 40%, even more preferably at least 60%, and most preferably at least 80%, where the transmittance at 425 nm in toluene is measured relative to toluene according to ASTM D1618-18.

[0220] The transmittance at 425 nm can be measured for the generated carbon black, and the quenching position can be adjusted until the transmittance of the generated carbon black at 425 nm is at least 20%, preferably at least 30%, more preferably at least 40%, even more preferably at least 60%, and most preferably at least 80%, where the transmittance at 425 nm in toluene is measured relative to toluene according to ASTM D1618-18.

[0221] The quenching position in the co-current reactor can be selected such that the transmittance of the produced carbon black at 425 nm is at least 20%, preferably at least 30%, more preferably at least 40%, even more preferably at least 60%, and most preferably at least 80%, where the transmittance at 425 nm in toluene is measured with respect to toluene in accordance with ASTM D1618-18.

[0222] Carbon black is included in many polymer compositions, for example, for modifying their color, mechanical, electrical, and / or processing properties. Carbon black is generally added, for example, to rubber compositions used to manufacture tires or their components to impart electrical dissipativity to the insulating matrix. At the same time, carbon black additives affect mechanical and elastic properties such as stiffness, abrasion resistance, and hysteresis, which greatly affect the performance of the resulting tires, for example, with respect to their rolling resistance and durability.

[0223] Reference will now be made to the accompanying drawings, which do not limit the scope and area of the present invention, to describe the present invention. The description provided is purely for the purpose of showing examples and explanatory diagrams. However, the specific features illustrated in the drawings may be used to further limit the scope of the present invention and the claims.

[0224] Figure 1 shows a furnace reactor (100) including a combustion chamber (101), a choke (102), and a tunnel (103). The reactor has an inner lining (106) and an outer lining (105). The combustion chamber (101) includes means for injecting fuel (101b) and oxygen-containing gas (101a). In the drawing, the oxygen-containing gas is injected into the combustion chamber (101) tangentially or radially via the oxygen-containing gas means (101a), and the fuel is injected axially into the combustion chamber (101) via the fuel injection means (101b). The oxygen-containing gas is preferably preheated to the temperatures described herein. The temperature of the high-temperature gas flow can be adjusted by preheating the oxygen-containing gas. Alternatively, the fuel can be preheated. In the combustion chamber (101), the fuel is burned in the presence of the oxygen-containing gas. After combustion, the temperature of the high-temperature carrier gas exceeds 800°C, bringing the particulate carbon-containing raw material to the temperature required for thermal decomposition. The particulate carbon-containing raw material can be injected directly into the combustion chamber (101), the choke (102), or the tunnel (103). The particulate carbon-containing raw material can also be injected in any of the aforementioned combinations, such as the choke (102) and the tunnel (103). The furnace reactor (100) includes several positions (104a, 104b, 104c, 104d) for quenching. The quenching agent, usually water, lowers the temperature of the high-temperature gas stream (or product mixture) so that the carbon black formation reaction is completed. Therefore, the quenching position affects the residence time of the raw material and components derived from the raw material. This means that adjusting the quenching position downstream of the reactor results in longer residence times. For example, quenching near the choke (102) (104a) results in a short residence time, while quenching downstream of the reactor (104c) results in a long residence time. The reaction volume is the volume of the reactor between the raw material injection point and the quenching point. When the raw material is injected into tunnel (103), the distance between the quenching point and the raw material injection point is 4200 mm, and the diameter of the tunnel is 200 m, the resulting reaction volume is 132 L. The feed rate of the particulate carbon-containing raw material should be adjusted according to the reaction volume, as described herein.In this invention, a rapid cooling position at the rear of the tunnel is particularly preferred so that the particulate carbon-containing raw material has sufficient time for evaporation or thermal decomposition.

[0225] Referring to Figure 2, a feed mixer (200) is shown, which includes a carrier gas inlet (204), a particle inlet (201), means for accelerating and injecting the carrier gas flow (207), a deagglutination conduit (209), a mixing chamber (206), and an outlet (210) for the carrier gas entrained with particles. Figure 2 also shows a carrier gas passage (212), which extends along the longitudinal axis through the feed mixer. The carrier gas (203) enters the feed mixer (200) through the carrier gas inlet (204) and is accelerated within means (207) to accelerate and inject the carrier gas flow. In Figure 2, the means for accelerating and injecting the carrier gas flow (207) is configured as a Laval nozzle. The Laval nozzle includes a convergence region (207a) in the direction of flow. The resulting carrier gas injection is injected into the mixing chamber (206). Particles, such as particulate carbon-containing raw material (202), are injected vertically into the mixing chamber (206). Thus, the particles are entrained in the accelerated carrier gas. The rapid acceleration of the particles leads to deagglomeration of the particles. The accelerated carrier gas containing the particles is further injected into the deagglomeration conduit (209). In the deagglomeration conduit (209), the particles collide with each other or with the inner wall or surface of the deagglomeration conduit (209), thereby achieving further deagglomeration. The means for accelerating and injecting the carrier gas flow (207) is preferably configured so that the carrier gas injection is directly injected into the deagglomeration conduit (209). This minimizes velocity loss. The deagglomeration conduit (209) typically includes, from downstream to upstream (in the flow direction), an inlet funnel (209a), a conduit (209b) with a constant inner diameter, and a diffusion nozzle (209c) that extends in the flow direction. The inlet funnel (209a) further enables optimal flow behavior into a conduit (209b) having a constant inner diameter. A diffusion nozzle (209c) that expands in the direction of flow is also beneficial to the flow behavior. The outlet (406) can be connected to means for injecting raw materials into the reactor as shown in Figure 1. Preferably, one feed mixer (200) supplies the deagglomerated raw materials to multiple means for injecting raw materials into the reactor. The feed mixer (200) more preferably includes a screw conveyor connected to the particle inlet (201).The screw conveyor can supply an appropriate amount or weight of particles into the mixing chamber (206). Furthermore, the feed mixer (200) can be operated under pressure such as 1.5 bar or 2 bar. A pressure tank for the particles (e.g., particulate carbon-containing raw material) can be installed. Such a pressure tank is fluidly connected to the particle inlet (201) and preferably connected to the feed mixer (200) via a valve. Preferably, two pressure tanks are present, with the first pressure tank connected to the second pressure tank. Both pressure tanks can be connected via a valve.

[0226] Figure 3 shows a Laval nozzle (300) for use in a feed mixer (200). A carrier gas passage (306) extends along the longitudinal axis through the Laval nozzle (300). Carrier gas (304) enters the Laval nozzle (300) and is accelerated. The carrier gas injection (305) then exits the Laval nozzle (300). The Laval nozzle (300) includes a section (301) with a constant diameter, a section (302a) converging in the direction of flow (302), a throat (303a), and a diverging section (303). In the Laval nozzle (300), the carrier gas is accelerated to a velocity greater than 1 Ma.

[0227] In addition, the present invention will be described in the following aspects.

[0228] Embodiment 1. A feed-mixing apparatus for supplying and mixing particles to a reactor, comprising: (i) a carrier gas passage extending through the feed-mixing apparatus; (ii) at least one carrier gas inlet having fluid communication with the carrier gas passage; (iii) at least one particle inlet; (iv) a mixing chamber having fluid communication with the at least one particle inlet and the carrier gas inlet; (v) a deagglutinating conduit having fluid communication with the mixing chamber; (vi) at least one outlet for the carrier gas encompassing the particles supplied to the mixing chamber, the at least one outlet having fluid communication with the deagglutinating conduit; and (vii) means for accelerating and injecting a carrier gas flow into the mixing chamber.

[0229] Embodiment 2. The supply mixing apparatus according to Embodiment 1, wherein the gas passage extends along the longitudinal axis passing through the supply mixing apparatus, and preferably the at least one inlet, mixing chamber, deagglutination conduit, and outlet are arranged along the longitudinal axis.

[0230] Embodiment 3. A supply and mixing apparatus according to any one of the preceding embodiments, wherein the particle inlet is configured to supply particles into the mixing chamber at an angle to the carrier gas injection released into the mixing chamber, preferably perpendicular to the carrier gas injection.

[0231] Embodiment 4. A feed-mixing apparatus according to any one of the preceding embodiments, wherein the means for accelerating and injecting the carrier gas flow includes at least one injection nozzle.

[0232] Embodiment 5. A feed-mixing apparatus according to any one of the preceding embodiments, wherein the means for accelerating and injecting the carrier gas flow extends from the at least one carrier gas inlet toward the at least one outlet and converges in the direction of flow.

[0233] Embodiment 6. A supply mixing apparatus according to either Embodiment 4 or 5, wherein the injection nozzle is a Laval nozzle.

[0234] Embodiment 7. A feed mixing apparatus according to any one of Embodiments 4 to 6, wherein the injection nozzle includes a converging section, a throat, and a diverging section.

[0235] Embodiment 8. A feed mixing apparatus according to any one of Embodiments 4 to 7, wherein the injection nozzle includes a diverging section, the angle of which is 2 to 30°, preferably 3 to 20°, more preferably 4 to 15°, and most preferably 5 to 10°.

[0236] Embodiment 9. A feed mixing apparatus according to any one of Embodiments 4 to 8, wherein the injection nozzle includes a converging section, the maximum inner diameter of the converging section being 5 to 50 mm, preferably 8 to 40 mm, more preferably 10 to 30 mm, and most preferably 12 to 20 mm.

[0237] Embodiment 10. A feed mixing apparatus according to any one of Embodiments 7 to 9, wherein the minimum inner diameter of the converging section and the diverging section and / or the inner diameter of the throat is 0.6 to 30 mm, preferably 1.2 to 18 mm, more preferably 1.9 to 12 mm, and most preferably 3 to 9 mm.

[0238] Embodiment 11. The feed mixing apparatus according to Embodiment 10, wherein the minimum inner diameter of the converging section and the diverging section and the inner diameter of the throat are the same.

[0239] Embodiment 12. A feeding and mixing apparatus according to any one of Embodiments 4 to 11, wherein the injection nozzle includes a diverging section, the maximum inner diameter of the diverging section being 0.3 to 11 mm, preferably 0.5 to 7 mm, more preferably 0.9 to 5 mm, and most preferably 1.1 to 4 mm.

[0240] Embodiment 13. A feed mixing apparatus according to any one of Embodiments 4 to 12, wherein the minimum inner diameter of the converging section is greater than the maximum inner diameter of the converging section, and preferably the difference between the maximum inner diameters of the converging section and the diverging section is 5 to 30 mm, preferably 8 to 20 mm, more preferably 9 to 18 mm, and most preferably 10 to 15 mm.

[0241] Embodiment 14. A feed mixing apparatus according to any one of Embodiments 4 to 13, wherein the maximum inner diameter of the converging section is greater than the maximum inner diameter of the diverging section.

[0242] Embodiment 15. A supply mixing apparatus according to any one of Embodiments 4 to 13, wherein the distance between the means for accelerating and injecting and the conduit having a constant inner diameter is 2 to 20 mm, preferably 2.5 to 15 mm, more preferably 3 to 10 mm, and most preferably 3.5 to 7 mm.

[0243] Embodiment 16. A supply mixing apparatus according to any one of the preceding embodiments, wherein the deagglutination conduit includes a conduit having a constant inner diameter.

[0244] Embodiment 17. A feed mixing apparatus according to any one of the preceding embodiments, wherein the deagglomeration conduit includes an inlet funnel, a conduit having a constant inner diameter, and a diffusion nozzle that extends in the direction of flow, from downstream to upstream.

[0245] Embodiment 18. A supply mixing apparatus according to any one of the preceding embodiments, wherein the longitudinal axis of the deagglutination conduit is coaxial with the longitudinal axis of the supply mixing apparatus.

[0246] Embodiment 19. A supply mixing apparatus according to any one of Embodiments 16 to 18, wherein the inner diameter of the conduit having a certain inner diameter is 1 to 20 mm, preferably 2 to 10 mm, more preferably 3 to 7 mm, and most preferably 4 to 6 mm.

[0247] Embodiment 20. A supply mixing apparatus according to any one of Embodiments 16 to 19, wherein the maximum inner diameter of the diffusion nozzle is greater than the inner diameter of a conduit having a constant inner diameter.

[0248] Embodiment 21. A feed mixing apparatus according to any one of Embodiments 17 to 20, wherein the maximum inner diameter of the diffusion nozzle is 5 to 50 mm, preferably 8 to 40 mm, more preferably 10 to 30 mm, and most preferably 12 to 20 mm.

[0249] Embodiment 22. A feed mixing apparatus according to any one of Embodiments 17 to 21, wherein the diffusion nozzle and the converging section of the injection nozzle have the same maximum inner diameter.

[0250] Embodiment 23. A feed mixing apparatus according to any one of Embodiments 16 to 22, wherein the angle of the diffusion nozzle is 1 to 30°, preferably 2 to 20°, more preferably 3 to 15°, and most preferably 4 to 8°.

[0251] Embodiment 24. A feed mixing apparatus according to any one of Embodiments 17 to 23, wherein the angle of the inlet funnel is 20 to 80°, preferably 30 to 75°, more preferably 40 to 70°, and most preferably 50 to 65°.

[0252] Embodiment 25. A feed mixing apparatus according to any one of Embodiments 17 to 20, wherein the maximum inner diameter of the diffusion nozzle is 5 to 50 mm, preferably 8 to 40 mm, more preferably 10 to 30 mm, and most preferably 12 to 20 mm.

[0253] Embodiment 26. A supply mixing apparatus according to any one of Embodiments 16 to 25, wherein the length of the conduit having a constant inner diameter is 3 to 500 mm, preferably 5 to 200 mm, more preferably 10 to 50 mm, and most preferably 13 to 30 mm.

[0254] Embodiment 27. A feed mixing apparatus according to any one of Embodiments 16 to 26, wherein the length of the diffusion nozzle is 10 to 300 mm, preferably 20 to 200 mm, more preferably 25 to 150 mm, and most preferably 30 to 100 mm.

[0255] Embodiment 28. A supply mixing apparatus according to any one of Embodiments 16 to 27, wherein the inner diameter of the conduit having a constant inner diameter is greater than the maximum inner diameter of the outlet of the means for accelerating and injecting the carrier gas flow.

[0256] Embodiment 29. A feed-mixing apparatus according to any one of the preceding embodiments, wherein means for accelerating and injecting a carrier gas flow, a mixing chamber and a deagglutinating conduit are configured such that the carrier gas injection is discharged into the deagglutinating conduit.

[0257] Embodiment 30. A supply mixing apparatus according to any one of the preceding embodiments, wherein the deagglutination conduit is configured as a diffusion tube.

[0258] Embodiment 31. A feed-mixing apparatus according to any one of the preceding embodiments, further comprising at least one hopper upstream of the at least one particle inlet.

[0259] Embodiment 32. A feed-mixing apparatus according to any one of the preceding embodiments, further comprising at least one screw conveyor upstream of the at least one particle inlet.

[0260] Embodiment 33. A feed-mixing apparatus according to any one of the preceding embodiments, wherein the particles are particulate carbon-containing raw materials and the reactor is a co-flow reactor for carbon black production.

[0261] Embodiment 34. A feed mixing apparatus according to any one of the preceding embodiments, further comprising a pressure tank for particles, the pressure tank being in fluid communication with the at least one particle inlet and optionally in communication with the at least one screw conveyor.

[0262] Embodiment 35. A reactor system comprising a reactor and a feed mixing device described in any one of the preceding embodiments, wherein the feed mixing device described in any one of the preceding embodiments is in fluid communication with the reactor.

[0263] Embodiment 36. The reactor system according to Embodiment 35, wherein the supply mixing device is preferably connected to a plurality of inlets of the reactor by an injection lance.

[0264] Embodiment 37. The reactor system according to any one of Embodiments 35 or 36, wherein the reactor is a co-flow reactor and the feed mixer is in fluid communication with a tunnel upstream of the choke, combustion chamber, and / or quenching region of the co-flow reactor.

[0265] Embodiment 38. The reactor system according to any one of Embodiments 35 to 37, wherein the reactor is a co-flow reactor, preferably a furnace reactor.

[0266] Embodiment 39. A method for injecting particulate matter into a reactor, comprising the steps of (a) deaggregating and entraining the particles into a carrier gas stream, preferably using a feed mixing device described in any one of Embodiments 1 to 34, and (b) injecting the carrier gas stream containing the deaggregated particles obtained in step (a) into the reactor.

[0267] Embodiment 40. The method according to Embodiment 39, wherein the method is for producing carbon black, the particulate material is a particulate carbon-containing raw material, and the reactor is a co-flow reactor for producing carbon black, preferably a furnace reactor.

[0268] Embodiment 41. The method according to Embodiment 40, wherein the particulate carbon-containing raw material is injected into a co-flow reactor by a plurality of inlets, preferably by a plurality of injection lances.

[0269] Embodiment 42. The method according to any one of Embodiments 39 to 41, wherein the carrier gas flow is accelerated and flows through a mixing chamber to a deagglutinating conduit.

[0270] Embodiment 43. The method according to any one of Embodiments 39 to 42, wherein deagglutination is performed by accelerating particles in a carrier gas stream and causing the particles to collide with the inner surface of a deagglutination conduit.

[0271] Embodiment 44. The method according to any one of Embodiments 39 to 43, wherein the carrier gas is accelerated to more than 1 Ma, preferably 1.01 Ma to 1.7 Ma, more preferably 1.1 Ma to 1.6 Ma, and most preferably 1.2 Ma to 1.5 Ma.

[0272] Embodiment 45. The method according to any one of Embodiments 39 to 44, wherein the particles are subjected to carrier gas injection perpendicular to the carrier gas injection.

[0273] Embodiment 46. The method according to any one of Embodiments 39 to 45, wherein the carrier gas stream containing deaggregated particles is injected into the reactor at a pressure of 0.5 bar to 2 bar, preferably 0.7 bar to 1.5 bar, more preferably 0.8 to 1.3 bar, and most preferably 0.8 to 1.2 bar.

[0274] Embodiment 47. The method according to any one of Embodiments 39 to 46, wherein the carrier gas further comprises H2O and / or an additive.

[0275] Embodiment 48. The method according to any one of Embodiments 39 to 46, wherein the carrier gas further comprises 1 to 10 volume percent of H2O.

[0276] Embodiment 49. Use of a feed-mixing apparatus according to any one of Embodiments 1 to 34 for deaggregating particles, preferably particulate carbon-containing raw materials. [Examples]

[0277] Example 1: Rubber granules The experiment in Example 1 is carried out in a small furnace reactor, as shown in Figure 1. The furnace reactor includes a combustion chamber, a choke, and a tunnel. The choke reduces the diameter to 45 mm. Downstream of the choke, a reactor tunnel is installed, having a diameter of 200 mm and a length of 4200 mm.

[0278] As shown in Figure 2, rubber granules were injected into the chalk of a furnace reactor via a feed mixer with a nozzle. The reaction volume of the reactor was approximately 130 liters. The reaction volume was the volume of the reactor between the raw material injection position and the quenching position. The feed mixer deaggregated the rubber granules by accelerating the particulate carbon-containing raw material. The rubber granules used in the experiment, i.e., 0.0-0.5 mm (product code 005GUM), were procured from ESTATO Umweltservice GmbH (ESTATO) in Germany. These rubber granules were derived from old tires and contained synthetic rubber (SBR) and natural rubber (NR). The particle fractions are shown in Table 1. Furthermore, the weight-average particle size (Dw50) was approximately 400 μm, measured according to ASTM D1511-12 (2017). However, it is also possible to use different particulate carbon-containing raw materials such as plastic granules or biomass-based granules.

[0279] [Table 1]

[0280] Table 2 shows the properties of rubber granules from ESTATO.

[0281] [Table 2]

[0282] Furthermore, the rubber granules contain several metals at a mass fraction of approximately 300 ppm, such as zinc and iron.

[0283] Measurement of CHNS content using an elemental analyzer The mass fractions of carbon, hydrogen, nitrogen, and sulfur are measured using an elemental analyzer equipped with a thermal conductivity detector and an infrared detector. This analyzer is a fully automated instrument for the quantitative analysis of the above elements. The combustion tube temperature is raised to 1100°C and the reduction tube temperature is set to 850°C. First, a blank measurement is performed. The carbon peak area should be less than 50, the hydrogen peak area less than 300, the nitrogen peak area less than 50, and the sulfur peak area less than 350. If not, the individual adsorption columns are heated and the blank measurement is restarted. The blank measurement is calculated as follows:

number

[0284] The compensation for blank measurements is calculated as follows: acomp.=ab Here, acomp. is the corrected peak area, a is the measured peak area, and b is the blank measurement value.

[0285] Next, the daily coefficient is measured. For this purpose, 3 mg of sulfanilamide and 3 mg of a low-level standard (e.g., carbon black standard) are weighed into eight tin capsules, respectively. After weighing each sample, they are placed in a capsule press, passed through with helium for 35 seconds, and then cryogenically sealed. After subtracting the blank value, the known theoretical elemental concentrations of the standard samples are correlated with the actually calculated elemental concentrations. As a result, the daily coefficient should be between 0.9 and 1.1. If not, these measurements should be repeated using newly opened standard solutions. Otherwise, a new calibration should be performed according to the manufacturer's instructions.

[0286] The daily coefficient is calculated as follows:

number

[0287] Next, eight tin capsules containing 5 mg ± 1 mg each of the desired measurement component, such as rubber granules, are weighed. After weighing each sample, they are placed in a capsule press, covered with helium for 35 seconds, and then cold-pressed.

[0288] For the measurement, the combustion tube is concentrated using O2. Elements C, H, N, and S burn to form CO2, H2O, NOx, SO2, and SO3. Halogens bound to the sample react to form volatile halogen compounds. Furthermore, WO3 particles are present in the combustion tube, supplying additional O2 as a catalyst, preventing the formation of non-volatile sulfates, and adsorbing interfering alkali and alkaline earth elements. The carrier gas stream is supplied to a Cu-filled reduction tube. Nitrogen oxides (NOx) are completely reduced to N2 upon contact with Cu. SO3 is reduced to SO2. Volatile halogen compounds are bound to silver wool.

[0289] N2 is not adsorbed and enters the thermal conductivity detector as the first measured component, while CO2, H2O, and SO2 are adsorbed onto their respective adsorption columns.

[0290] Next, the adsorption column is sequentially heated to its desorption temperature, and CO2, then H2O, is introduced as carrier gases into a thermal conductivity detector, followed by SO2 into an infrared detector. Depending on the type and concentration of the components, the detectors deliver digitized and integrated electrical signals. The measurement signals are recorded as a function of time and displayed as integral values. The absolute elemental content of the sample is calculated from these integral values ​​and calibration coefficients for each individual measurement peak.

[0291] Elemental concentrations are calculated according to the following formula.

number

[0292] Measurement of O content using an elemental analyzer Depending on the oxygen concentration, an electrical signal is transmitted from the thermal conductivity detector (WLD) of the elemental analyzer to a microcontroller, where it is then displayed as an integrated value. The absolute elemental content of the sample was determined from the integrated value of the measured peak and the calibration coefficient. The pyrolysis tube is heated to 1050°C. First, a blank measurement is performed. The oxygen peak area should have a maximum value of 200. If the blank value is not less than 200, the CO adsorption column needs to be heated (260°C, CO desorption 150°C). After the blank measurement is successful, the average value of the blank value range is calculated.

[0293] The blank measurement is calculated as follows:

number

[0294] Next, the daily coefficient is measured. For this purpose, 3 mg of acetanilide is weighed into each of eight tin capsules. After weighing each sample, it is placed in a capsule press, passed through with helium for 35 seconds, and then cryogenically sealed. After subtracting the blank value, the known theoretical elemental concentrations of the standard sample are correlated with the actually calculated elemental concentrations. As a result, the daily coefficient should be between 0.9 and 1.1. If this is not the case, these measurements should be repeated using a newly opened standard solution. Otherwise, a new calibration should be performed according to the manufacturer's instructions.

[0295] The daily coefficient is calculated as follows:

number

[0296] Next, eight tin capsules containing 5 mg ± 1 mg each of the desired measurement component, for example, rubber granules, are weighed. After weighing each sample, they are placed in a capsule press, covered with helium for 35 seconds, and then cold-pressed. The samples are then measured.

[0297] Elemental concentrations are calculated according to the following formula.

number

[0298] Reaction conditions in a furnace reactor

[0299] The reaction conditions for carbon black production are shown in Table 3. The temperature of the high-temperature gas flow after the injection of raw materials is calculated as described in the specification. As mentioned above, the temperature (absolute temperature) can also be measured using a pyrometer. Furthermore, the residence times of particles with diameters of 0.5 mm and 1 mm are calculated. A pyrolysis modeling program was used for the calculations.

[0300] [Table 3] 1 273.15K and 101325Pa 2 The k-value is defined by the ratio of the amount of stoichiometric O2 required for the complete stoichiometric combustion of the fuel to the amount of O2 supplied.

[0301] [Table 4]

[0302] After injecting the rubber granule raw material, the reaction was rapidly cooled with water, the resulting carbon black was dried, and pulverized to obtain a volume-average particle size of approximately 5 μm. The carbon black obtained according to the present invention (see Experiments A1-E12) was compared with standard carbon black N660 and recovered carbon black rCB. rCB was recovered from the thermal decomposition of rubber granules.

[0303] The temperature inside the combustion chamber, i.e., the temperature of the high-temperature combustion gas, was controlled by the temperature of the combustion air upstream of the combustion chamber (i.e., the temperature of the oxygen-containing gas). The k-value was controlled by the flow of natural gas (fuel) into the combustion chamber.

[0304] The resulting carbon black contains approximately 53% by weight recovered carbon black, approximately 27% by weight new carbon black, and approximately 20% by weight ash. The recovered carbon black contains coke. Since rubber granules are used in the co-flow reactor process, it is possible not only to recover carbon black but also to produce new carbon black derived from the rubber. Therefore, the ash content is lower compared to carbon black recovered from REOIL (RCB615, approximately 23.2% by weight ash). The ash content can be measured at 550°C for 16 hours according to ASTM D1506-99.

[0305] The carbon black obtained in each experiment was characterized, and the results are shown in Table 4.

[0306] [Table 5] 3 N550 Carbon black obtained from liquid raw materials, Orion Engineering Carbons Co., Ltd. 4 N660 Carbon black obtained from liquid raw materials, Orion Engineering Carbons Co., Ltd. 5 rCB 2 is a recycled carbon black, REOIL SPZO.O. 6 The aggregate size distribution was measured as described below. 7 The specific surface area (AGV) was measured as described below. 8 Volatile matter was measured at 950°C for 7 minutes, as described below. 9 The BET surface area was measured according to ASTM D6556-21. 10 STSA surface area was measured according to ASTM D6556-21. 11 Iodine adsorption was measured according to ASTM D1510-21. 12The pH value is measured according to ASTM D1512-21, Test Method B - Sonic Slurry. 13 The amount of oil absorbed by compression (COAN) was measured according to ASTM D3493-20 (using paraffin oil). 14 Oil absorption capacity (OAN) was measured according to ASTM D2414-19 (using paraffin oil). 15 The transmittance at 425 nm in toluene (transmittance of toluene extract) was measured relative to toluene according to ASTM D1618-18.

[0307] [Table 6]

[0308] Aggregate size distribution All test results are analyzed in accordance with ISO 15825:2016 using a Brookhaven BI-DCP disk centrifuge equipped with a red photodiode. The cited test results are provided to Brookhaven Software after appropriate parameter adjustments as described in ISO 185825:2017-03 “Computer and Software Setup”.

[0309] Specific surface area (AGV) The specific surface area of ​​the test sample is available in Brookhaven software. After testing the sample and reviewing the results, click "Details" and read the value "Specific Surface Area sq / g" on the computer display.

[0310] Volatile components at 950℃ The volatile content at 950°C was measured using a thermogravimetric analyzer (TGA-701) from Fa.LECO Instrumente, following the protocol below. The sample dish was dried at 650°C for 30 minutes. The carbon black material was stored in a desiccator with a desiccant before measurement. The dried sample dish was loaded into the instrument, its tare weight was measured, and it was filled with 0.5g to 10g of carbon black material. Next, the oven of the TGA instrument with the sample-filled dish loaded was gradually heated to 105°C by automatic software control, and the sample was dried until a certain mass was achieved. Subsequently, the dish was closed with a lid, the oven was purged with nitrogen (99.9 vol% grade), and heated to 950°C. The oven temperature was maintained at 950°C for 7 minutes. The volatile content at 950°C was calculated using the following formula.

number

[0311] result Surprisingly, it was found that particulate carbon-containing raw materials can be used in the co-current reactor process. As can be seen from Table 3, the resulting carbon has desirable properties compared to standard carbon black products obtained from liquid carbon-containing raw materials.

[0312] Furthermore, the aggregate size and surface area are smaller compared to those of the recovered carbon black. This indicates that the obtained carbon black has a lower coke content. The specific surface area measured by aggregate size further indicates the amount of coke present in the carbon black. Moreover, a high aggregate size is also an indicator of a high coke content.

[0313] Furthermore, as can be seen from Table 3, the residence time of A6 was 0.367 seconds, and the temperature of the high-temperature gas flow was 1763°C. Higher temperatures are thought to result in optimal residence times, which were 0.28 seconds for particles with a diameter of 0.5 mm and 1.05 seconds for particles with a diameter of 1 mm. The transmittance in experiment B9 using A6 was 95%. Transmittance is an indicator of the complete thermal decomposition of the raw material or the C,H-containing compounds in the raw material. Therefore, higher temperatures and longer residence times are considered beneficial for producing carbon black from particulate raw materials.

[0314] Example 2: Rubber composition

[0315] The preparation of rubber compositions and rubber testing are described below. General methods for the production of rubber compounds and their vulcanized products are described in the book "Handbook of Rubber Technology" by W. Hoffmann, Hanser Press, 1994.

[0316] The rubber compositions are listed in Table 5. ESBR Buna SB1500 was introduced into a Harburg Freudenberger laboratory mixer GK1.5E with a PES5 rotor shape and ground for 30 seconds at a chamber temperature of 40°C, a packing density of 0.66, and a rotor speed of 45 rpm. Subsequently, half the volume of carbon black, ZnO, and stearic acid were added under grinding. After 90 seconds, the remaining half of the volume of carbon black and 6 PPD were added. After another 90 seconds, the ram was lifted, washed, and the batch was mixed for a further 90 seconds. The total mixing time in the internal mixer was 5 minutes, after which the batch was dropped onto an open mill to cool and further distributed and mixed. The batch temperature did not exceed 160°C in the first mixing step. The batch was allowed to stand overnight.

[0317] Next, during the second final mixing step, sulfur and an accelerator (Vulkacit CZ / EG-Z) were added in the indicated amounts to the masterbatch obtained from the first mixing step. The resulting mixture was milled in a GK1.5E mixer for 2 minutes at a chamber temperature of 40 °C and a filling rate of 0.64. The rotor speed was 30 rpm, and the batch temperature was ensured not to exceed 110 °C. Finally, the mixture was removed from the internal mixer and reprocessed on an open mill. The resulting vulcanizable composition (green compound) was cured at a temperature of 165 °C for 11 to 15 minutes (C1: 15 minutes, C2: 12 minutes, C3: 12 minutes, C4: 12 minutes, C5: 11 minutes, C6: 12 minutes, C7: 12 minutes, C8: 11 minutes, C9: 11 minutes).

[0318]

Table 7

[0319] The properties of the test specimens were measured and the results are shown in Table 6. The results were compared with carbon black produced using liquid carbon black raw materials (N660 and N550), and the recovered carbon black rCB.

[0320]

Table 8

[0321] Relative peak area of ​​topography

[0322] The relative peak area of the topography is an indicator of the filler dispersion determined by the surface topography (including medallion correction), which follows the procedures described in A. Vermeyer, "Analysis of Filler Dispersion by Topography Measurement", Technical Report TR820, Degussa, and A. Vermeyer, "Development of a Method for Evaluating the Characteristics of Filler Dispersion in Rubber Mixtures Using Surface Topography", Master's Thesis, University of Applied Sciences Münster, 1998, and DE19917975C2.

[0323] Loss factor tan(d) The above values and the loss factor tan(d) were measured in accordance with DIN 53 513, in strain control mode (1 ± 0.5 mm) or force control mode (50 N ± 25 N), at 60 °C, frequency 16 Hz, using cylindrical test specimens (height 10 mm, diameter 10 mm).

[0324] result The examples demonstrate that carbon blacks produced according to the present invention (carbon blacks A3-A5, A8-A10) can be beneficially used in rubber compositions (experiments C5-C10). The resulting carbon blacks have a low loss factor tan(d) combined with high topography and high tensile strength. Furthermore, the elongation at fracture is advantageously 612-665%. The ball rebound of the resulting carbon blacks is equivalent to that of carbon blacks N660 and N550.

[0325] It will be understood that various modifications can be made without departing from the principles of the present invention, and that many changes can be made in preferred embodiments. [Explanation of symbols]

[0326] 100 reactors 101 Combustion Chamber 101a Oxygen-containing gas 101b Fuel 102 Chalk 103 Tunnel 105 Outer lining 106 Inner lining 200 Feed mixer 201 Particle Inlet 202 Particulate carbon-containing raw materials 203 Carrier gas 204 Carrier gas inlet 206 Mixing Chamber 207 Means for accelerating and injecting carrier gas flow 209 Deagglomeration conduit 212 Carrier gas passage

Claims

1. A particle supply and mixing device for a reactor, (i) A carrier gas passage extending through a supply mixing unit, (ii) At least one carrier gas inlet that is in fluid communication with the carrier gas passage, (iii) At least one particle inlet, (iv) A mixing chamber having fluid communication with at least one particle inlet and the carrier gas inlet, (v) A deagglomeration conduit that is in fluid communication with the mixing chamber, (vi) At least one outlet for a carrier gas encompassing particles supplied to the mixing chamber, comprising at least one outlet in fluid communication with a deagglutination conduit, (vii) A feed mixing apparatus comprising means for accelerating and injecting a carrier gas flow into a mixing chamber.

2. The supply and mixing apparatus according to claim 1, wherein the particle inlet is configured to supply particles into the mixing chamber at an angle to the carrier gas injection released into the mixing chamber, preferably perpendicular to the carrier gas injection.

3. The feed mixing apparatus according to claim 1 or 2, wherein the means for accelerating and injecting the carrier gas flow includes at least one injection nozzle, preferably a Laval nozzle.

4. The deagglomeration conduit includes an inlet funnel, a conduit having a constant inner diameter, and a diffusion nozzle that spreads in the direction of flow, from downstream to upstream, according to any one of claims 1 to 3.

5. The feed mixing apparatus according to any one of claims 1 to 4, further comprising at least one screw conveyor upstream of the at least one particle inlet.

6. The feed mixing apparatus according to any one of claims 1 to 5, wherein the particles are a carbon-containing raw material and the reactor is a co-flow reactor for carbon black production.

7. A reactor system comprising a reactor and a feed mixing device according to any one of claims 1 to 6, wherein the feed mixing device is in fluid communication with the reactor.

8. The reactor system according to claim 7, wherein the supply mixing device is preferably connected to a plurality of inlets of the reactor by an injection lance.

9. The reactor system according to claim 7 or 8, wherein the reactor is a co-flow reactor, preferably a furnace reactor.

10. A method for injecting particulate matter into a reactor, comprising the following steps: (a) Preferably by using a supply mixing device according to any one of claims 1 to 6, the steps include de-aggregating and entraining the particles in a carrier gas stream, (b) A step of injecting a carrier gas stream containing the deaggregated particles obtained in step (a) into the reactor.

11. The method according to claim 10, wherein the method is a method for producing carbon black, the particles are particulate carbon-containing raw materials, and the reactor is a co-flow reactor for producing carbon black, preferably a furnace reactor.

12. The method according to claim 11, wherein the particulate carbon-containing raw material is injected into a co-flow reactor by a plurality of inlets, preferably by a plurality of injection lances.

13. The method according to any one of claims 10 to 12, wherein the carrier gas flow is accelerated and flows through the mixing chamber to the deagglutination conduit, and / or the carrier gas is accelerated to more than 1 Ma, preferably 1.01 Ma to 1.7 Ma, more preferably 1.1 Ma to 1.6 Ma, and most preferably 1.2 Ma to 1.5 Ma.

14. Carrier gas is H ２ The gas further comprises O and / or additives, preferably the carrier gas being 1 to 10% by volume of H ２ The method according to any one of claims 10 to 13, further comprising O.

15. Use of a feed mixing apparatus according to any one of claims 1 to 6 for deaggregating particles, preferably particulate carbon-containing raw materials.

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