Carbon black from particulate raw materials

Abstract

This invention relates to a method for producing carbon black in a co-current reactor using a particulate carbon-containing raw material.

Description

[Technical Field]

[0001] This invention relates to a method for producing carbon black in a co-current reactor using a particulate carbon-containing raw material. [Background technology]

[0002] The production of carbon black involves the decomposition or thermal decomposition of carbon-containing raw materials in a reaction chamber at temperatures such as 800°C (e.g., in the temperature ranges of 1100°C and 2000°C). These high temperatures are obtained by the combustion of a mixture containing oxygen-containing gas and combustion fuel (i.e., fuel). The carbon black (CB) encombusted in the gas (high-temperature gas stream) exiting the reaction chamber is then cooled in a quenching step and subsequently collected by any preferred means conventionally used in the art.

[0003] Carbon black has many applications, including as a reinforcing or filler for the rubber and tire industries. Furthermore, its use is increasing in other areas, such as 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.

[0004] 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] In prior art, the feedstock for producing carbon black in a co-flow reactor, such as a furnace reactor, is limited to liquid carbon-containing feedstocks. Liquid carbon-containing feedstocks are, for example, liquid hydrocarbons, such as cracked oils derived from steam crackers or fluid catalytic cracking units.

[0006] Immediately after injecting the liquid carbon-containing raw material into the carbon black reactor, the raw material is evaporated to form carbon black. Since the conversion of particulate carbon-containing raw material to gaseous components is considerably slower compared to liquid carbon-containing raw material, achieving the desired thermal decomposition of particulate carbon-containing raw material is difficult.

[0007] As an alternative approach, particulate carbon-containing raw materials, such as tires, can be pyrolyzed in a pyrolysis reactor. The pyrolysis is carried out at low temperatures, such as 500°C, yielding liquid, gaseous, and solid fractions. The liquid fraction can then be used to produce new or unused carbon black (nCB) in a co-flow reactor, such as a furnace reactor.

[0008] U.S. Patent Application Publication No. 2002 / 0117388 relates to the aforementioned pyrolysis of scrap rubber materials, including old tires. The object of U.S. Patent Application Publication No. 2002 / 0117388 is to recover components in scrap rubber materials, such as carbon black. After pyrolysis, carbon black can be recovered from the pyrolysis gas (recovered carbon black, "rCB").

[0009] However, the solid yield from thermal decomposition at low temperatures is low, and a subsequent manufacturing process is required to obtain carbon black from the liquid fraction of the thermal decomposition. Furthermore, the coke and ash content of the carbon black recovered after thermal decomposition is undesirable.

[0010] Therefore, a new method for producing carbon black that allows the use of particulate carbon-containing raw materials should be developed. Surprisingly, we found that particulate carbon-containing raw materials can be used in a co-flow reactor where the high-temperature gas flow has a temperature of at least 800°C. [Overview of the project]

[0011] This objective is achieved by 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, the method comprising (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, the high-temperature gas flow having a temperature of at least 800°C.

[0012] Furthermore, carbon black produced according to the method of the present invention is provided, as well as a composition comprising (A) an elastomer polymer material and (B) carbon black obtained according to the present invention, and an article produced from or comprising the composition of the present invention.

[0013] Furthermore, the following carbon black will be provided. (I) BET surface area is 80-90m 2 The value is / g, and preferably the BET surface area is 85-88m². 2 The pressure absorption rate is 58-69 mL / 100g, preferably 61-64 mL / 100g, and preferably the STSA surface area is 72-82 m². 2 The value is / g, and more preferably the STSA surface area is 76-79 m². 2 Carbon black having a density of / g, preferably with a volatile content of 2.1-2.7% by weight, more preferably with a volatile content of 2.3-2.5% by weight, preferably with a transmittance of more than 50% at 425nm in toluene, more preferably with a transmittance of more than 77% at 425nm in toluene; where the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured using paraffinic oil according to ASTM D3493-20, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (II) BET surface area is 70-85m 2 The value is / g, and preferably the BET surface area is 77-79m². 2 / g, with an oil absorption under compression of 59 to 70 mL / 100 g, preferably an oil absorption under compression of 63 to 65 mL / 100 g, preferably an STSA surface area of 68 to 78 m 2 / g, more preferably an STSA surface area of 71 to 73 m 2 / g, preferably an oil absorption under compression of 58 to 69 mL / 100 g, more preferably an oil absorption under compression of 63 to 65 mL / 100 g, preferably a volatile content of 2.0 to 2.6% by weight, more preferably a volatile content of 2.2 to 2.4% by weight, preferably a transmittance at 425 nm in toluene of over 40%, more preferably a transmittance at 425 nm in toluene of over 56% carbon black; where the BET surface area is measured according to ASTM D6556-21, the oil absorption under compression is measured using paraffinic oil according to ASTM D3493-20, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950 °C for 7 minutes as described in the specification, and the transmittance at 425 nm in toluene is measured according to ASTM D1618-18 with respect to toluene; and / or (III) a BET surface area of 80 to 96 m 2 / g, preferably a BET surface area of 89 to 92 m 2 / g, with an oil absorption under compression of 60 to 69 mL / 100 g, preferably an oil absorption under compression of 63 to 65 mL / 100 g, preferably an STSA surface area of 79 to 87 m 2 / g, more preferably an STSA surface area of 82 to 84 m 2Carbon black having a density of / g, preferably with a volatile content of 2.2-2.9% by weight, more preferably with a volatile content of 2.5-2.7% by weight, preferably with a transmittance of more than 40% at 425nm in toluene, more preferably with a transmittance of more than 62% at 425nm in toluene; where the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured using paraffinic oil according to ASTM D3493-20, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (IV) BET surface area is 120-138 m² 2 The value is / g, and preferably the BET surface area is 127-130m². 2 The pressure absorption capacity is 58-69 mL / 100g, preferably 62-64 mL / 100g, and preferably the STSA surface area is 82-95 m². 2 The value is / g, and more preferably the STSA surface area is 87-89 m². 2 Carbon black having a density of / g, preferably with a volatile content of 2.6-3.2% by weight, more preferably with a volatile content of 2.8-3.0% by weight, preferably with a transmittance of more than 60% at 425nm in toluene, more preferably with a transmittance of more than 80% at 425nm in toluene; where the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured according to ASTM D3493-20 using paraffinic oil, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (V) BET surface area is 82-95m 2 The value is / g, and preferably the BET surface area is 86-89m². 2 The pressure absorption capacity is 59-70 mL / 100g, preferably 63-65 mL / 100g, and preferably the STSA surface area is 70-82 m². 2The value is / g, and more preferably the STSA surface area is 76-78m². 2 Carbon black having a density of / g, preferably with a volatile content of 1.8-2.4% by weight, more preferably with a volatile content of 2.0-2.2% by weight, preferably with a transmittance of more than 60% at 425nm in toluene, more preferably with a transmittance of more than 80% at 425nm in toluene; where the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured according to ASTM D3493-20 using paraffinic oil, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425nm in toluene is measured relative to toluene according to ASTM D1618-18.

[0014] In addition, particulate carbon-containing raw materials are used for the production of carbon black in co-flow reactors.

[0015] Furthermore, a method is provided for adjusting the quenching position in a co-flow reactor for producing carbon black from particulate carbon-containing raw materials, the method comprising: I) injecting the particulate carbon-containing raw materials into a high-temperature gas stream of a co-flow reactor, where the high-temperature gas stream has a temperature of at least 800°C; II) quenching the high-temperature gas stream containing the produced carbon black; III) measuring the transmittance of the produced carbon black; and III) adjusting the quenching position in the co-flow reactor until the transmittance of the produced carbon black 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%, with the transmittance at 425 nm in toluene measured against toluene according to ASTM D1618-18. [Brief explanation of the drawing]

[0016] [Figure 1] Cross-section of a furnace reactor

[0017] [Figure 2] Feed mixing device with nozzle

[0018] [Figure 3] Laval nozzle for feed mixing device

[0019] [Figure 4] Deagglutination conduit for supply mixing device

[0020] [Figure 5] Nozzle-less supply and mixing device [Modes for carrying out the invention]

[0021] 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.

[0022] 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.

[0023] The term "raw material" refers to the raw materials supplied for the production of carbon black. According to the present invention, particulate raw materials are used in the production of carbon black. As used herein, the term or abbreviation "raw material" refers to particulate carbon-containing raw materials.

[0024] 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.

[0025] 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 itself 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.

[0026] 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.

[0027] The present invention relates to 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, the method comprising (a) providing a high-temperature gas flow, (b) providing a particulate carbon-containing raw material, and (d) injecting the particulate carbon-containing raw material into the high-temperature gas flow to form carbon black, the high-temperature gas flow having a temperature of at least 800°C.

[0028] 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.

[0029] 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.

[0030] Accordingly, the present invention can be described as 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, the method 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.

[0031] Particulate carbon-containing raw materials can include inert compounds, coke, C,H-containing compounds, and / or carbon black, preferably carbon black and C,H-containing compounds. 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 atm. In methods for producing carbon black, it is preferable not to use liquid carbon-containing raw materials in the production of carbon black.

[0032] Generally, the raw materials used in carbon black production are particulate carbon-containing materials.

[0033] Particulate 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.

[0034] 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.

[0035] 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.

[0036] 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 C,H-containing compounds, more preferably 30 to 90% by weight of C,H-containing compounds, and most preferably 40 to 70% by weight of C,H-containing compounds, based on the total weight of the particulate carbon-containing raw material.

[0037] The particulate carbon-containing raw material may contain inert compounds, which may include metals, metallic compounds, silicon, and silica. The metals may be zinc, silicon, calcium, aluminum, and / or iron.

[0038] 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.

[0039] The particulate carbon-containing raw 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 raw 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 raw material. Alternatively, the particulate carbon-containing raw material may not contain recovered carbon black.

[0040] In this context, recovered carbon black refers to recoverable carbon black in this method. In other words, it is carbon black present in the raw materials that is not produced by the method of the present invention.

[0041] C,H-containing compounds are, for example, rubber, plastics, and / or biomass-based materials. The particulate carbon-containing raw material is preferably provided as granules (i.e., carbon-containing granular raw material). Therefore, the particulate carbon-containing raw material may include rubber granules, plastic granules, and / or biomass-based granules, or all of them. 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 include carbon black.

[0042] 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 / 12 The carbon-to-carbon ratio is lower in fossil fuels compared to biomass fuels. Therefore, fossil fuels are sources in which the relative amount of C14 atoms compared to C12 is lower than that of naturally occurring (or bio-based) sources.

[0043] 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 60-80% by weight, based on the total weight of the particulate carbon-containing raw material.

[0044] Preferably, the amount of particulate 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.

[0045] 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.

[0046] 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.

[0047] Particulate biomass-based carbon black raw materials may include wood, grass, cellulose, hemicellulose, lignin, and / or natural rubber.

[0048] 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.

[0049] 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 or particulate carbon-containing raw materials may be derived from tires, cable sheaths, tubes, conveyor belts, shoe soles, hoses, or mixtures thereof.

[0050] 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.

[0051] 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.

[0052] The plastic granules are preferably derived from household waste materials, such as plastic bags, plastic containers, and plastic packaging.

[0053] The raw material is preferably provided in granular form. This can be achieved by grinding to a desired particle size or granule size. For example, tires can be ground to obtain granular rubber granules as a raw material.

[0054] 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).

[0055] 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).

[0056] 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).

[0057] 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).

[0058] 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).

[0059] 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).

[0060] 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).

[0061] 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.

[0062] 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.

[0063] 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.

[0064] 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).

[0065] 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).

[0066] 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).

[0067] 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.

[0068] 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).

[0069] 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).

[0070] 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).

[0071] 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).

[0072] The particle size distribution range of the particulate carbon-containing raw material (Dw90-Dw10) / Dw50 may be 0.2 to 1.8, preferably 0.3 to 1.3, more preferably 0.4 to 1.1, and most preferably 0.4 to 1.0, where the particle size distributions Dw10, Dw50, and Dw90 are measured according to ASTM D1511-12 (2017).

[0073] 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.

[0074] 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.

[0075] Carbon black (including rCB) and / or particulate carbon-containing raw materials manufactured in accordance with the present invention 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). The carbon black of the present invention 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). The carbon black of the present invention can have a pMC (modern carbon content) of 100% as measured according to ASTM D6866-20 Method B (AMS).

[0076] 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 according to the present invention.

[0077] The mass flow rate of the raw materials should be adjusted so that the raw materials are heated uniformly. The particulate carbon-containing raw material 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.

[0078] The fuel may include gaseous or liquid hydrocarbons, preferably natural gas, fuel oil, or H2.

[0079] 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.

[0080] 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.

[0081] 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.

[0082] 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 generally 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.

[0083] 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.

[0084] 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.

[0085] 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".

[0086] 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.

[0087] 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.

[0088] 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.

[0089] Oxygen-containing gases and fuels can be preheated electrically or using heat exchangers.

[0090] Water affects the surface properties of the carbon black produced. Therefore, the amount of oxygen-containing gas, such as O2, in the combustion mixture can be used to control the amount of water in the high-temperature combustion mixture and / or high-temperature reaction mixture, thereby preferably controlling the surface properties of the carbon black produced.

[0091] The tunnel is 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.

[0092] 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).

[0093] 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.

[0094] The particulate carbon-containing raw material should be injected through multiple inlets, preferably radially and perpendicularly to the central longitudinal axis of the reactor.

[0095] The concentration of O2 in the high-temperature gas stream should be less than 5 volume%, preferably less than 4 volume%, more preferably 0.01 to 3 volume%, and most preferably 0.1 to 2 volume%.

[0096] The resulting carbon black generally contains both recovered carbon black and new carbon black.

[0097] 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 gas flow, 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.

[0098] 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).

[0099] 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.

[0100] 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.

[0101] 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.

[0102] 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.

[0103] 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.

[0104] 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), can be sprayed into the tunnel to stop the carbon black reaction at the appropriate time and place.

[0105] 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 to 100% by weight, preferably 50 to 99% by weight, more preferably 60 to 95% by weight, and most preferably 70 to 90% by weight, where the weight percentage is based on the total weight of the oxygen-containing gas.

[0106] The tubular conduit can have a cylindrical shape that extends along the central longitudinal axis of the reactor without curving.

[0107] 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.

[0108] 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.

[0109] 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.

[0110] The oxygen-containing gas is generally supplied in an amount that produces an excess of oxygen relative to the amount of oxygen required for the complete combustion of the fuel, and / or the oxygen-containing gas is supplied in an amount such that 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 amount of stoichiometric O2 required for the complete stoichiometric combustion of the fuel to the amount of O2 supplied.

[0111] The flow rates of the fuel and oxygen-containing gas can be adjusted to achieve high temperatures, usually kept close to the stoichiometric ratio. The ratio must be adjusted to prevent the melting of the refractory material. The range of oxygen-containing flow is very wide, for example, about 1000 Nm³. 3 From the lowest / h, approximately 100kNm 3 Up to high values ​​per hour, for example, 1000 Nm 3 / h~100kNm 3 / h, 1000Nm 3 / h~10kNm 3 / h, 2000Nm 3 / h~3000Nm 3 / h, or 1000Nm 3 / h~2000Nm 3 The values ​​are / h. However, the present invention is not limited to these amounts, and larger reactors require higher airflows, while smaller reactors require lower airflows.

[0112] The desired temperature of the high-temperature gas flow can also be achieved by plasma heating the gas flow. The gas flow can be preheated as described above.

[0113] 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 2500°C to 20,000°C. The plasma carrier gas can be oxygen or hydrogen. Hydrogen is particularly preferred as the plasma carrier gas.

[0114] 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).

[0115] 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.

[0116] 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

[0117] Volumetric flow rate is the volume of fluid per unit second after 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

[0118] 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.

[0119] 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.

[0120] 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.

[0121] 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. The residual oxygen from the combustion does not result in complete combustion. Therefore, it is presumed that CO and H2O with the same CO / H2O ratio are formed according to the C / H ratio of the raw materials.

[0122] The reaction temperature can be calculated from the energy balance.

number

[0123] 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. uFThis 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 O2 This 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 expressed as follows. The corresponding mass flow rate is mp i The lower heating value of this compound is shown as H ui This is shown. When a raw material containing particles is transported into the reactor along with a gas flow, this 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 generation. Heat loss is Q Loss This is considered by the mass flow rate of the hydrocarbon portion of the particulate carbon, which is m R It can be expressed as follows and calculated using the following formula.

number

[0124] 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 wAnd, based on the assumption of total oxidation of gaseous water as a reaction product, the following equation is obtained.

number

[0125] A is an unoxidized substance. f p = fe. The amount of heat generated is as follows:

number

[0126] 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

[0127] Molar heat capacity can be found using the same textbook, such as "Properties of Gases and Liquids" or the NIST Data Book.

[0128] When the fuel consists of more than one type, the lower heating value can be determined by the following formula.

number

[0129] 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.

[0130] The difference in thermal enthalpy of fuels containing more than one type of fuel is calculated using the following formula.

number

[0131] The average molecular weight of the fuel is determined by the following formula.

number

[0132] 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.

[0133] 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

[0134] 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 equation.

number

[0135] The lower heat of release of inert species in the product stream is set to 0 J / mol.

[0136] 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.

[0137] The lower heating value of particulate raw materials is calculated using the following formula.

number

[0138] 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 particles is determined by the following formula.

number

[0139] The C / H ratio of the hydrocarbon portion can be obtained from the final analysis of the particulate raw material and the final analysis of the Conradson.

number

[0140] The molar enthalpy difference of water can be determined by the following formula.

number

[0141] In the case of CO2, it can be obtained by the following formula.

number

[0142] In the case of SO2

number

[0143] In the case of N2

number

[0144] In the case of O2

number

[0145] In the case of CO

number

[0146] The lower heating value of CO is H u,CO = 282980 J / mol.

[0147] In the case of gaseous rubber products

number

[0148] In the case of particulate rubber, it can be obtained by the following formula.

number

[0149] In Conradson's case

number

[0150] Calculation example

[0151] Combustion of methane entering the combustion chamber at a temperature of 3 bar and T=290K.

[0152] 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. 3Let's use / h(STP).

[0153] 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.

[0154] 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)

[0155] Therefore, we obtain h_f by the following equation.

number

[0156] 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.

[0157] 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).

[0158] 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.

[0159] Calculation of the mass flow rate of the compound in the reaction region

[0160] 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 the total oxygen flow rate, which is obtained by subtracting the oxygen flow rates in the form of CO2 and H2O (SO2 if sulfur is present in the fuel). The conversion between mass flow rate and standard volume flow rate for a gas species is performed by the following formula.

number

[0161] Therefore, the remaining oxygen flow rate is obtained.

number

[0162] 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.

[0163] 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

[0164] 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

[0165] Conradson is treated as an inert material, calculated as follows:

number

[0166] Calculation of heat loss

[0167] The heat flux can be calculated using the following formula.

number

[0168] In the case of free convection α, it is calculated as a function of the Rayleigh number and the Prandtl number Pr, given by the Nusselt number.

number

[0169] Using the following formula,

number

[0170] The Rayleigh number is calculated using the following formula:

number

[0171] Integrating all of these into an energy balance yields the following equation:

number

[0172] The reactor is 15.9 m 2 It has an external surface area of ​​. Therefore, in this example, the temperature is 1629°C. The reaction volume is 0.162 m³. 3 The volumetric flow rate for all species except Micro-Conradson is 1236 m³. 3 It is / h. Therefore, the residence time is obtained by the following equation,

number

[0173] 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.

[0174] The formation of carbon black is generally terminated by rapid cooling of a high-temperature gas stream. Therefore, the method may further include a step of rapidly cooling the high-temperature gas stream after injection in step (d).

[0175] 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.

[0176] The transmittance at 425 nm can be measured for the produced carbon black, and the quenching position can be adjusted until 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 against toluene in accordance with ASTM D1618-18.

[0177] The quenching position in the entrained flow 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 against toluene in accordance with ASTM D1618-18.

[0178] Furthermore, a method for adjusting the quenching position in an entrained flow reactor for producing carbon black from a particulate carbon-containing raw material is provided, the method comprising: I) injecting the particulate carbon-containing raw material into a high-temperature gas stream in the entrained flow reactor, where the high-temperature gas stream has a temperature of at least 800 °C; II) quenching the high-temperature gas stream containing the produced carbon black; II) measuring the transmittance of the produced carbon black; III) adjusting the quenching position in the entrained flow reactor until the transmittance of the produced carbon black 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 against toluene in accordance with ASTM D1618-18.

[0179] It is particularly preferred that the particulate carbon-containing raw material is deagglomerated before injection into the reactor. The evaporation time is thought to be reduced by using deagglomerated particles.

[0180] Therefore, step (b) further includes deflocculating the particulate carbon-containing raw material, and in step (d), it is desirable to inject the deflocculated particulate carbon-containing raw material into a high-temperature gas stream to form carbon black.

[0181] And a method for producing carbon black from a particulate carbon-containing raw material in a co-current reactor having a flow path along the central longitudinal axis of the reactor should be provided. This method includes (a) providing a high-temperature gas stream, (b) deflocculating the particulate carbon-containing raw material to provide a deflocculated particulate carbon-containing raw material, and (d) injecting the deflocculated particulate carbon-containing raw material into the high-temperature gas stream to form carbon black, wherein the high-temperature gas stream has a temperature of at least 800 °C.

[0182] Deflocculation can be achieved by (i) accelerating the particulate carbon-containing raw material and / or (ii) preferably applying a shear force using an extruder. Deflocculation can be carried out (i) preferably in a feed mixing device including a nozzle and / or (ii) in an extruder. The feed mixing device is preferably a device according to the present invention.

[0183] Acceleration of the particulate carbon-containing raw material results in deflocculation 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, deflocculation can be carried out by subjecting the particulate carbon-containing raw material to carrier gas injection.

[0184] Deflocculation can be carried out (i) in a feed mixing device including a Laval nozzle.

[0185] The carrier gas and / or the particulate carbon-containing raw material is preferably 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. A Mach number exceeding 1 can be achieved using an injection nozzle such as a Laval nozzle. Ma is the Mach number.

[0186] 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.

[0187] 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 of particulate carbon-containing material and a surface such as the inner surface of a deaggregation conduit.

[0188] The deaggregated particulate carbon-containing raw material (or carrier gas containing the deaggregated particulate carbon-containing raw material) 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. As described above, the pressure should be adjusted according to the injection position of the raw material. 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 raw material, or carrier gas containing the deaggregated particulate carbon-containing raw material, should be injected into the combustion chamber at a higher pressure.

[0189] The deaggregated particulate carbon-containing raw material can be included in a carrier gas, which further contains H2O and / or additives. H2O can prevent the reaggregation of particles in the carrier gas. Therefore, the deaggregated particulate carbon-containing raw material should be included in a carrier gas, which may further contain H2O in an amount of 1 to 10 volume%, preferably 2 to 8 volume%, and more preferably 3 to 7 volume%, based on the total volume of the carrier gas containing the deaggregated particulate carbon-containing raw material.

[0190] Particulate carbon-containing raw materials and / or de-aggregated carbon-containing raw materials are generally contained in the carrier gas.

[0191] Deagglutination can be carried out in a device for supplying and mixing particles to 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 in fluid communication with the carrier gas passage; (iii) at least one particle inlet; (iv) a mixing chamber in fluid communication with the at least one particle inlet and the carrier gas inlet; (v) a deagglutination conduit in 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 in fluid communication with the deagglutination conduit; and (vii) means for accelerating and injecting the carrier gas flow into the mixing chamber.

[0192] The gas passage should extend along the longitudinal axis of the supply mixing device, preferably with at least one inlet, mixing chamber, deagglutination conduit, and outlet located along the longitudinal axis.

[0193] 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.

[0194] 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.

[0195] The injection nozzle can 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, in the following order, a nozzle including a converging section, a throat, and a diverging section accelerates the gas flow.

[0196] The cross-sectional area is typically circular or elliptical at each point of the spray nozzle.

[0197] The spray nozzle may include a divergence 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°.

[0198] 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.

[0199] 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.

[0200] 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.

[0201] 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.

[0202] The minimum inner diameter of the converging section must be larger than the maximum inner diameter of the converging section. Preferably, the difference between the maximum inner diameters of the converging section and the diverging section is 5 - 30 mm, preferably 8 - 20 mm, more preferably 9 - 18 mm, and most preferably 10 - 15 mm.

[0203] The maximum inner diameter of the converging section may be larger than the maximum inner diameter of the diverging section.

[0204] The distance between the means for accelerating and injecting the carrier gas and the conduit having a constant inner diameter can be 2 - 20 mm, preferably 2.5 - 15 mm, more preferably 3 - 10 mm, and most preferably 3.5 - 7 mm. The specific distance between the aforementioned components improves the deaggregation of the particles because the injection flow directly flows into the disaggregation conduit. Therefore, turbulent flow can be avoided and the loss of the velocity of the injection flow is minimized.

[0205] The means (or nozzle) for accelerating and injecting the carrier gas may be arranged such that the means for accelerating and injecting the carrier gas protrudes into the cavity of the inlet funnel of the disaggregation conduit.

[0206] The disaggregation conduit usually includes a conduit having a constant inner diameter. In a conduit having a constant inner diameter, the particles collide with each other or the particles collide with the wall of the conduit having a constant inner diameter and are further disaggregated. The disaggregation conduit can be configured as a diffuser tube.

[0207] The disaggregation conduit can include, from downstream to upstream, an inlet funnel, a conduit having a constant inner diameter, and a diffuser nozzle that expands in the flow direction. The diverging nozzle should continuously increase the inner diameter of the disaggregation conduit. Therefore, the carrier gas flow is not interrupted and turbulent flow is avoided. The angle of the diffuser nozzle can be 1 - 30°, preferably 2 - 20°, more preferably 3 - 15°, and most preferably 4 - 8°. The angle of the inlet funnel can be 20 - 80°, preferably 30 - 75°, more preferably 40 - 70°, and most preferably 50 - 65°.

[0208] 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.

[0209] 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 deaggregation. Therefore, the diameter should be selected for a specific particulate material, preferably for the mass flow rate.

[0210] 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.

[0211] The focusing sections of the diffusion nozzle and the injection nozzle can have the same maximum inner diameter.

[0212] 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.

[0213] 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.

[0214] 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.

[0215] 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.

[0216] 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.

[0217] The supply mixing device may further include at least one hopper upstream of the at least one particle inlet.

[0218] 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.

[0219] The particles described in the feed mixing apparatus are particulate carbon-containing raw materials, and the reactor is typically a co-flow reactor used for carbon black production.

[0220] 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.

[0221] 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.

[0222] 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.

[0223] A method for injecting particulate matter into a reactor can be provided, comprising the steps of (a) deaggregating and entraining the particles in a carrier gas stream, preferably by using a feed mixing device, and (b) injecting the carrier gas stream containing the deaggregated particles obtained in step (a) into the reactor.

[0224] This method can be used to produce carbon black, where 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.

[0225] The particulate carbon-containing raw material can be injected into the co-flow reactor through multiple inlets, preferably through multiple injection lances.

[0226] The carrier gas flow can be accelerated and flow through the mixing chamber into the deagglutination conduit.

[0227] 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.

[0228] The carrier gas is generally accelerated to 1 Ma or higher, 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.

[0229] The particles can be directed perpendicularly to the carrier gas injection and used for the carrier gas injection.

[0230] The carrier gas stream containing 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.

[0231] 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.

[0232] The supply and mixing device can be used to deaggregate particles, preferably particulate carbon-containing raw materials.

[0233] Furthermore, carbon black manufactured according to the method of the present invention is provided. The carbon black may include new carbon black and recovered carbon black.

[0234] Carbon black is included in many polymer compositions, for example, to modify their color, mechanical, electrical, and / or processing properties. For example, carbon black is commonly added to rubber compositions used to manufacture tires or their components to impart electrical dissipation to the insulating matrix. At the same time, carbon black additives affect mechanical and elastic properties such as stiffness, wear resistance, and hysteresis, which greatly influence the performance of the resulting tire, for example, in terms of its rolling resistance and durability.

[0235] The present invention provides a composition comprising (A) an elastomer polymer material and (B) carbon black obtained according to the present invention. It should be noted that articles derived from the above composition can also be used as raw materials.

[0236] The term “composition,” as used herein, refers to a material composed of multiple constituent chemical species or components. “Elastomer polymer material” is understood to be a material consisting essentially of elastomer polymers. The term “polymer” is used herein in its general sense in the art, referring to a high molecular weight compound, i.e., a compound having a relatively high molecular weight (e.g., 500 Da or more), whose structure contains multiple repeating units (also called “mers”) that are actually or conceptually derived from chemical species of relatively low molecular weight. The term “elastomer polymer” is used herein in its general sense in the art, referring to an elastic polymer.

[0237] Particularly useful as elastomer polymer materials (or elastomer polymer materials) for carrying out the present invention are elastomers such as rubber materials. The elastomer polymer material (a) of the composition according to the present invention may include one or more types of rubber. The terms “rubber,” “rubber material,” and “elastomer” may be used interchangeably throughout this specification unless otherwise specified. Rubbers that can be used in accordance with the present invention include those containing olefinic unsaturated rubbers, i.e., diene rubber materials, as well as non-diene rubber materials. The term “diene rubber material” is intended to include both natural rubber and synthetic rubber, or mixtures thereof. The elastomer polymer material (a) may consist of synthetic rubber.

[0238] The elastomer polymer material (A) of the composition according to the present invention may include natural and / or synthetic rubber.

[0239] Natural rubber can be used in its raw form and in various processed forms conventionally known in the field of rubber processing. Natural rubber can be obtained, for example, from rubber trees (Helvia brasiliensis), guayule, and dandelion. Therefore, the elastomer polymer material (A) may contain or consist of natural rubber.

[0240] Examples of synthetic rubbers include styrene-butadiene rubbers 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 thereof. According to the present invention, synthetic rubber can also be obtained from renewable materials. For example, polybutadiene can be produced from alcohol obtained by the fermentation of plant biomass.

[0241] Suitable rubbers may also include functionalized rubbers and rubbers bonded to silicon or tin. For example, rubbers can be functionalized with functional groups such as amines, alkoxys, silyls, thiols, thioesters, thioethers, sulfanyls, mercaptos, sulfides, or combinations thereof. One or more functional groups may be primary, secondary, or tertiary and may be located at one or both chain ends (e.g., α,ω-functionalization), may be suspended from the polymer backbone, and / or provided within the polymer backbone. The rubbers according to the present invention may also be partially crosslinked. Therefore, before use in compositions of the present invention, a portion of the polymer chains of the rubber material may be crosslinked with or without a coupling agent.

[0242] The compositions according to the present invention may be curable compositions, such as vulcanizable rubber compositions. The term "vulcanizable rubber composition" refers to a composition of rubber components that can be cured by vulcanization in the presence of a vulcanized product, and which optionally contains various further components conventionally used in the art of rubber compounding. The terms "curable" and "vulcanizable" are used interchangeably throughout this specification unless otherwise specified, and refer to a chemical reaction that links polymer chains together with a crosslinking agent or vulcanizing agent. The curing reaction can be induced by any means known in the art, such as light, moisture, heat and / or the addition of a crosslinking agent.

[0243] The elastomer polymer material (A) according to the present invention may include natural rubber. According to the present invention, the natural rubber may include natural rubber obtained from rubber trees (Helvia brasiliensis), guayule, dandelion, or a mixture of any combination thereof. The natural rubber may include natural rubber obtained from guayule and / or dandelion. The elastomer polymer material (A) may include natural rubber with a content of 5 phr or more, for example, 10 phr or more, or 15 phr or more, or 20 phr or more, or 30 phr or more, or 40 phr or more, or 50 phr or more, or 60 phr or more, or 70 phr or more, or 80 phr or more. As used herein, the term "phr" refers to parts by weight of each listed individual material per 100 parts by weight of rubber or elastomer. The elastomer polymer material (A) may contain natural rubber with a ferrous oxide content of 100 phr or less, for example, 95 phr or less, or 90 phr or less, or 85 phr or less, or 80 phr or less, or 75 phr or less, or 70 phr or less, or 65 phr or less, or 60 phr or less. The elastomer polymer material (A) may contain natural rubber in a range between any of the above lower and upper limits. For example, the elastomer polymer material (A) may contain natural rubber in the range of 5 to 95 phr, for example, 10 to 90 phr, or 20 to 80 phr, or 30 to 70 phr, or 40 to 60 phr. According to the present invention, the elastomer polymer material (A) may consist of natural rubber.

[0244] The elastomer polymer material (A) according to the present invention may include synthetic rubber. According to the present invention, the synthetic rubber may include synthetic rubber obtained from renewable materials. The renewable material according to the present invention may be an alcohol obtained by fermentation of plant biomass. For example, the synthetic rubber may include polybutadiene obtained from an alcohol obtained by fermentation of plant biomass. The elastomer polymer material (A) may include synthetic rubber with a phr of 5 phr or more, for example, 10 phr or more, or 15 phr or more, or 20 phr or more, or 30 phr or more, or 40 phr or more, or 50 phr or more, or 60 phr or more, or 70 phr or more, or 80 phr or more. As used herein, the term "phr" refers to parts by weight of each listed individual material per 100 parts by weight of rubber or elastomer. The elastomer polymer material (A) may include synthetic rubber with a ferrous ratio of 100 phr or less, for example, 95 phr or less, or 90 phr or less, or 85 phr or less, or 80 phr or less, or 75 phr or less, or 70 phr or less, or 65 phr or less, or 60 phr or less. The elastomer polymer material (A) may include synthetic rubber in a range between any of the above lower and upper limits. For example, the elastomer polymer material (A) may include synthetic rubber in the range of 5 to 95 phr, for example, 10 to 90 phr, or 20 to 80 phr, or 30 to 70 phr, or 40 to 60 phr. According to the present invention, the elastomer polymer material (A) may consist of synthetic rubber.

[0245] According to the present invention, the elastomer polymer material (A) may include a mixture of natural rubber and synthetic rubber. The elastomer polymer material (A) may include natural rubber of 5-100 phr and synthetic rubber of 5-100 phr, for example, natural rubber of 10-90 phr and synthetic rubber of 10-90 phr, or natural rubber of 20-80 phr and synthetic rubber of 20-80 phr, or natural rubber of 30-70 phr and synthetic rubber of 30-70 phr, or natural rubber of 40-60 phr and synthetic rubber of 40-60 phr, or natural rubber of 40-100 phr and synthetic rubber of 5-60 phr, or natural rubber of 50-95 phr and synthetic rubber of 5-50 phr, or natural rubber of 60-90 phr and synthetic rubber of 10-50 phr, or natural rubber of 5-40 phr and synthetic rubber of 60-100 phr, or natural rubber of 10-20 phr and 80-90 phr. For example, the elastomer polymer material (A) may contain 50 phr of natural rubber and 50 phr of synthetic rubber, or the elastomer polymer material (A) may contain 5 phr of natural rubber and 95 phr of synthetic rubber.

[0246] The synthetic rubber according to the present invention preferably comprises emulsion-styrene-butadiene rubber (ESBR), polybutadiene, polyisoprene, butyl rubber, halogenated butyl rubber, or a mixture of any combination thereof, more preferably polyisoprene and / or polybutadiene, and even more preferably polybutadiene. The synthetic rubber according to the present invention preferably comprises emulsion-styrene-butadiene rubber (ESBR), polybutadiene, polyisoprene, butyl rubber, halogenated butyl rubber, or a mixture of any combination thereof, more preferably polyisoprene and / or polybutadiene, and even more preferably polybutadiene. The synthetic rubber may contain emulsion-styrene-butadiene rubber (ESBR), polybutadiene, polyisoprene, butyl rubber, halogenated butyl rubber, or a mixture of any combination thereof, preferably polyisoprene or polybutadiene, and more preferably polybutadiene. Synthetic rubber may contain or consist of polybutadiene, polyisoprene, butyl rubber, halogenated butyl rubber, or a mixture of any of these, preferably polyisoprene or polybutadiene, more preferably polybutadiene.

[0247] The generated carbon black can also be pulverized before being added to the composition. Therefore, the composition may contain pulverized carbon black.

[0248] The composition may include carbon black (B) obtained according to the present invention in a concentration of 3 to 200 phr, preferably 5 to 190 phr, more preferably 10 to 150 phr, even more preferably 20 to 130 phr, and most preferably 30 to 100 phr.

[0249] The composition may include one or more additives selected from vulcanizing agents, curing aids such as primary and secondary vulcanization accelerators, activators and pre-vulcanization inhibitors, processing additives such as oils, waxes, resins, plasticizers, softeners, rheology modifiers, pigments, mixing accelerators, coupling agents, surfactants, biocides, and anti-degradation agents such as heat or light stabilizers, antioxidants and ozone inhibitors, metal oxides, metal hydroxides, and fillers such as silica, organosilica, carbon nanotubes, carbon fibers, graphite and metal fibers.

[0250] The compositions of the present invention can be obtained and processed by general elastomer processing techniques. For example, the compositions according to the present invention can be obtained by combining the carbon black material (B) and optional components (if used) of the present invention with an elastomer polymer (A), mixing them, and dispersing the carbon black material (B) and optional components (if used) in the elastomer polymer (A). Dispersion can be achieved by any means known in the art, such as mixing, stirring, grinding, kneading, ultrasonic, dissolving, shaker mixer, rotor stirring dispersion assembly or high-pressure homogenizer or a combination thereof. For example, a laboratory mixer having a meshing rotor shape can be used. Dispersion can be carried out, for example, until the carbon black (B) is uniformly dispersed in the elastomer polymer material (A) and the dispersion index is 95% or higher, preferably 97% or higher, or 99% or higher, according to ASTM D2663-88 Test Method B.

[0251] The composition according to the present invention can be prepared, for example, by a multi-step process: First, carbon black (B) and optionally non-curable additives (if used) can be added simultaneously or sequentially to an elastomer polymer material (A). The elastomer polymer material (A), carbon black (B), and additives (if used) can then be mixed at a temperature typically in the range of 40°C to 160°C for a total mixing time of less than 10 minutes, for example, in the range of 2 to 8 minutes. Subsequently, the resulting mixture can be blended with one or more curable additives at a temperature below 115°C for less than 5 minutes, typically less than 3 minutes, preferably about 2.5 minutes.

[0252] The method may include further steps such as extruding the product or cooling it to room temperature and storing it for further processing. The method may further include a curing step, which can be carried out by subjecting the composition to thermosetting conditions, for example, a temperature of 120-200°C for 5 minutes to 3 hours. Curing can be carried out, for example, in a curing press at a temperature of 140-180°C for 5 to 60 minutes at a pressure of 100-150 bar.

[0253] As can be understood, the compositions according to the present invention can be used in a variety of technical applications requiring polymer-based materials containing carbon black fillers to impart, for example, antistatic or conductive properties, color, mechanical reinforcement, and / or low hysteresis properties. Mechanical properties of particular interest in tire manufacturing include tear resistance, resilience, and hysteresis. The compositions according to the present invention provide cured compositions having good and beneficial mechanical properties, particularly for tire manufacturing. Beneficial mechanical properties according to the present invention include, for example, high tensile strength, high resilience, and low hysteresis. The compositions according to the present invention provide cured compositions having mechanical properties comparable to conventional rubber compositions containing carbon black.

[0254] Accordingly, the present invention also relates to articles, particularly tires, made from or containing the aforementioned compositions according to the present invention. A tire according to the present invention may include a tread, carcass, sidewall, inner liner, apex, shoulder, hump strip, chafer, and / or bead filler, at least one of which is made from or contains the compositions according to the present invention. Examples of such tires, but not limited to, include truck tires, passenger car tires, off-road tires, aircraft tires, agricultural tires, and earthmoving tires. The tire and / or tire components described may also be used as rubber granules.

[0255] The tire may include a sidewall, the sidewall being made from a composition according to the present invention, the composition preferably comprising (A) 40-60 phr of natural rubber and 40-60 phr of synthetic rubber, preferably 50-60 phr of natural rubber and 40-50 phr of synthetic rubber, more preferably 55 phr of natural rubber and 45 phr of synthetic rubber, where the synthetic rubber preferably comprises polybutadiene, more preferably polybutadiene, and (B) 30-70 phr of carbon black, preferably 40-60 phr, comprising a tread, carcass, sidewall, inner liner, apex, shoulder, hump strip, chafer, and / or bead filler, where at least carbon black, preferably 50 phr of carbon black.

[0256] The tire may include a carcass, which is made from a composition according to the present invention, the composition preferably comprising (A) 40-80 phr of natural rubber and 20-60 phr of synthetic rubber, preferably 50-70 phr of natural rubber and 30-50 phr of synthetic rubber, more preferably 60 phr of natural rubber and 40 phr of synthetic rubber, and (B) 5-70 phr of carbon black, preferably 40-60 phr of carbon black, more preferably 50 phr of carbon black, where the synthetic rubber preferably comprises polybutadiene and emulsion-styrene-butadiene rubber (ESBR), more preferably 20 phr of polybutadiene and 20 phr of emulsion-styrene-butadiene rubber (ESBR).

[0257] The tire includes a chafer, which is made from a composition according to the present invention, the composition preferably comprises (A) 30-70 phr of natural rubber and 30-70 phr of synthetic rubber, preferably 40-60 phr of natural rubber and 40-60 phr of synthetic rubber, more preferably 50 phr of natural rubber and 50 phr of synthetic rubber, and (B) 55-95 phr of carbon black, preferably 65-85 phr of carbon black, more preferably 75 phr of carbon black, where the synthetic rubber preferably comprises emulsion-styrene-butadiene rubber (ESBR), more preferably emulsion-styrene-butadiene rubber (ESBR).

[0258] The tire may include a bead filler and / or apex, the bead filler and / or apex being made from a composition according to the present invention, the composition preferably comprising (A) 80-100 phr of natural rubber, preferably 90-100 phr of natural rubber, more preferably 100 phr of natural rubber, and (B) 35-75 phr of carbon black, preferably 45-65 phr of carbon black, more preferably 55 phr of carbon black.

[0259] The tire may include an inner liner, which is made from a composition according to the present invention, the composition preferably comprising (A) 80-100 phr of synthetic rubber, preferably 90-100 phr of synthetic rubber, more preferably 100 phr of synthetic rubber, and (B) 40-80 phr of carbon black, preferably 50-70 phr of carbon black, more preferably 60 phr of carbon black, where the synthetic rubber preferably comprises halogenated butyl rubber, more preferably halogenated butyl rubber.

[0260] The tire may include a tread, preferably a truck tire, and the tread is made from a composition according to the present invention, the composition preferably comprises (A) 60-95 phr of natural rubber and 5-40 phr of synthetic rubber, preferably 70-85 phr of natural rubber and 15-30 phr of synthetic rubber, more preferably 80 phr of natural rubber and 20 phr of synthetic rubber, and (B) 30-70 phr of carbon black, preferably 40-60 phr of carbon black, more preferably 50 phr of carbon black, where the synthetic rubber preferably comprises polybutadiene, more preferably polybutadiene.

[0261] The tire may include a tread, preferably a passenger car tire, and the tread is made from a composition according to the present invention, the composition preferably comprises (A) 80-100 phr of synthetic rubber, preferably 90-100 phr of synthetic rubber, more preferably 100 phr of synthetic rubber, and (B) 35-75 phr of carbon black, preferably 45-65 phr of carbon black, more preferably 55 phr of carbon black, where the synthetic rubber preferably comprises solution-styrene-butadiene rubber (SSBR) and polybutadiene, more preferably 70 phr of solution-styrene-butadiene rubber (SSBR) and 30 phr of polybutadiene.

[0262] The tire may include a tread, preferably a passenger car tire, and the tread is made from a composition according to the present invention, the composition preferably comprises (A) 80-100 phr of synthetic rubber, preferably 90-100 phr of synthetic rubber, more preferably 100 phr of synthetic rubber, (B) 35-75 phr of carbon black, preferably 45-65 phr of carbon black, more preferably 55 phr of carbon black, and (C) 60-100 phr of silica, preferably 70-90 phr of silica, more preferably 80 phr of silica, where the synthetic rubber preferably comprises solution-styrene-butadiene rubber (SSBR) and polybutadiene, more preferably 70 phr of solution-styrene-butadiene rubber (SSBR) and 30 phr of polybutadiene.

[0263] The tire may include a tread, preferably an off-road (OTR) tire, the tread being made from a composition according to the present invention, the composition preferably comprising (A) 80-100 phr of natural rubber, preferably 90-100 phr of natural rubber, more preferably 100 phr of natural rubber, and (B) 35-75 phr of carbon black, preferably 45-75 phr of carbon black, more preferably 55 phr of carbon black.

[0264] The articles may be cable sheaths, tubes, drive belts, conveyor belts, roll covers, shoe soles, hoses, sealing components, profiles, damping elements, coatings, or colored or printed articles.

[0265] Furthermore, the article may be a conveyor belt, which is made from the composition according to the present invention, and the composition preferably comprises (A) 60-95 phr of natural rubber and 5-40 phr of synthetic rubber, preferably 70-85 phr of natural rubber and 15-30 phr of synthetic rubber, more preferably 80 phr of natural rubber and 20 phr of synthetic rubber, and (B) 30-70 phr of carbon black, preferably 40-60 phr of carbon black, more preferably 50 phr of carbon black, where the synthetic rubber preferably comprises polybutadiene, more preferably polybutadiene.

[0266] Furthermore, the present invention relates to the use of the above-mentioned compositions for manufacturing tires, preferably pneumatic tires, tire treads, belts, belt reinforcements, carcasses, carcass reinforcements, sidewalls, inner liners, apex, shoulders, hump strips, chafers, bead fillers, cable sheaths, tubes, drive belts, conveyor belts, roll covers, soles, hoses, sealing members, profiles, damping elements, coatings, or colored or printed articles.

[0267] Furthermore, the present invention uses a deaggregated particulate carbon-containing raw material for the production of carbon black in a co-flow reactor.

[0268] The present invention will now be described with reference to the accompanying drawings, which do not limit the scope and domain of the invention. The description provided is purely for illustrative purposes and illustrative purposes. However, certain features illustrated in the drawings may be used to further limit the scope and claims of the invention.

[0269] 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.

[0270] 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.

[0271] 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.

[0272] Figure 4 shows a deagglutination conduit (400) for use in a feed mixer (200). A carrier gas passage (407) extends along the longitudinal axis through the deagglutination conduit (400). The deagglutination conduit (400) includes an inlet funnel (401), a conduit (402) having a constant inner diameter, and a diffusion nozzle (403a) that expands in the direction of flow (403a). Furthermore, an outlet (404) is shown which can be connected to means for injecting deagglutination particles (e.g., deagglutinated particulate carbon-containing particles) (406) into the reactor.

[0273] Figure 5 shows an alternative feed mixer (500). Figure 5 also shows a carrier gas passage (506). The carrier gas passage (506) extends along the longitudinal axis through the feed mixer. The feed mixer (500) comprises an inlet (504) for the carrier gas (501), a mixing chamber (505), an inlet (502) for particles, and an outlet (503). The carrier gas (501) enters the feed mixer (500). The carrier gas (501) should have a desirable velocity such as less than 1 Ma, or 2 m / s to 1 Ma, or 20 m / s to 200 m / s. Particles, such as particulate carbon-containing feedstock (202), are injected vertically into the mixing chamber (507). Thus, the particles are entrained in the accelerated carrier gas. Rapid acceleration of the particles leads to deaggregation of the particles. The outlet (503) can be connected to a reactor. Similar to the supply mixing unit (200), a screw conveyor and at least one pressure tank can be installed.

[0274] In addition, the present invention will be described in the following aspects.

[0275] Embodiment 1. A method for producing carbon black from a particulate carbon-containing raw material in a co-flow reactor having a flow channel along the central longitudinal axis of the reactor, (a) To provide a high-temperature gas flow, (b) To provide a raw material containing particulate carbon, and (d) The process includes injecting particulate carbon-containing raw materials into a high-temperature gas stream to form carbon black, A method in which a high-temperature gas stream has a temperature of at least 800°C.

[0276] Embodiment 2. The method according to Embodiment 1, wherein step (b) further comprises deaggregating a particulate carbon-containing raw material, and in step (d), the deaggregated particulate carbon-containing raw material is injected into a high-temperature gas stream to form carbon black.

[0277] Embodiment 3. A method for producing carbon black from a particulate carbon-containing raw material in a co-flow reactor having a flow channel along the central longitudinal axis of the reactor, (a) To provide a high-temperature gas flow, (b) De-aggregating a particulate carbon-containing raw material to provide a de-aggregated particulate carbon-containing raw material, and (d) The process includes injecting the deaggregated particulate carbon-containing raw material into a high-temperature gas stream to form carbon black, A method in which a high-temperature gas stream has a temperature of at least 800°C.

[0278] Embodiment 4. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material comprises an inert compound, coke, a C,H-containing compound, and / or carbon black, preferably ash and carbon black.

[0279] Embodiment 5. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material further comprises an inert compound, the inert compound comprising zinc, silicon, calcium, aluminum, and / or iron.

[0280] Embodiment 6. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material comprises 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.

[0281] Embodiment 7. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material further contains carbon black, the carbon black present in the particulate carbon-containing raw material in an amount of 1 to 70% by weight, preferably 2 to 50% by weight, more preferably 5 to 40% by weight, and most preferably 10 to 30% by weight, based on the total weight of the particulate carbon-containing raw material.

[0282] Embodiment 8. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material comprises 10 to 100% by weight of a C,H-containing compound, preferably 20 to 99% by weight of a C,H-containing compound, more preferably 30 to 90% by weight of a C,H-containing compound, and most preferably 40 to 70% by weight of a C,H-containing compound, based on the total weight of the particulate carbon-containing raw material.

[0283] Embodiment 9. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material includes rubber granules, plastic granules, and / or biomass-based granules.

[0284] Embodiment 10. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material contains rubber granules, and the rubber granules contain carbon black.

[0285] Embodiment 11. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material includes an aggregated raw material.

[0286] Embodiment 12. The method according to any one of the preceding embodiments, wherein 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 of particulate carbon-containing raw material 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, the particle size being measured according to ASTM D1511-12 (2017).

[0287] Embodiment 13. The method according to any one of the preceding embodiments, wherein the particle size distribution of the particulate carbon-containing raw material is measured according to ASTM D1511-12(2017), (a) Sieve number 10 holds 1 to 0 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 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 particulate carbon-containing raw material, and / or (c) Sieve number 35 holds 10-80% by weight, preferably 15-70% by weight, more preferably 20-60% by weight, and most preferably 25-55% by weight of particulate carbon-containing raw material, and / or (d) Sieve number 60 holds 5-70% by weight, preferably 10-60% by weight, more preferably 15-50% by weight, most preferably 20-45% by weight of particulate carbon-containing raw material, and / or (e) Sieve number 120 holds 1 to 80% by weight, preferably 7 to 70% by weight, more preferably 5 to 60% by weight, most preferably 7 to 50% by weight of particulate carbon-containing raw material, and / or (f) A method wherein the bottom tray contains particulate carbon-containing raw material in an amount of less than 4% by weight, preferably less than 3% by weight, more preferably 0 to 2% by weight, and most preferably 0.01 to 1% by weight.

[0288] Embodiment 14. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material 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, having 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).

[0289] Embodiment 15. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material 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, having 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 the particle size is measured according to ASTM D1511-12 (2017).

[0290] Embodiment 16. The method according to any one of the preceding embodiments, wherein the 50% by weight cumulative particle size of the particulate carbon-containing raw material is 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 50% by weight cumulative particle size is measured according to ASTM D1511-12 (2017).

[0291] Embodiment 17. The method according to any one of the preceding embodiments, wherein the weight-average particle size Dw50 of the particulate carbon-containing raw material is 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).

[0292] Embodiment 18. The method according to any one of the preceding embodiments, wherein the particle size distribution Dw10 of the particulate carbon-containing raw material is 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).

[0293] Embodiment 19. The method according to any one of the preceding embodiments, wherein the particle size distribution Dw90 of the particulate carbon-containing raw material is 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).

[0294] Embodiment 20. The method according to any one of the preceding embodiments, wherein the particle size distribution range of the particulate carbon-containing raw material (Dw90-Dw10) / Dw50 is 0.2 to 1.8, preferably 0.3 to 1.3, more preferably 0.4 to 1.1, and most preferably 0.4 to 1.0, where the particle size distributions Dw10, Dw50 and Dw90 are measured according to ASTM D1511-12 (2017).

[0295] Embodiment 21. A method for producing carbon black, wherein liquid carbon-containing raw materials are not used in the production of carbon black, according to any one of the preceding embodiments.

[0296] Embodiment 22. The method according to any one of the preceding embodiments, wherein the high-temperature gas flow is obtained by electric preheating, plasma heating, and combustion of a fuel and oxygen-containing gas.

[0297] Embodiment 23. A method according to any one of the preceding embodiments, (a1) Fuel and oxygen-containing gas are supplied to the combustion chamber of the reactor, (b2) A high-temperature gas flow is generated by burning fuel in a combustion chamber. A method by which a high-temperature gas flow is generated.

[0298] Embodiment 24. The method according to any one of the preceding embodiments, wherein the co-current reactor is a furnace reactor.

[0299] Embodiment 25. The method according to any one of Embodiments 22 to 24, wherein the particulate carbon-containing raw material is injected into the combustion chamber, choke and / or tunnel of a furnace reactor, preferably into the choke of the furnace reactor.

[0300] Embodiment 26. The method according to any one of the preceding embodiments, wherein the high-temperature gas flow has 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.

[0301] Embodiment 27. The method according to any one of Embodiments 22 to 26, wherein the oxygen-containing gas is preheated to a temperature of 200 to 1600°C, preferably 350 to 1400°C, more preferably 500 to 1200°C, and most preferably 450 to 950°C.

[0302] Embodiment 28. The method according to any one of Embodiments 22 to 27, wherein the fuel is preheated to a temperature of 50 to 750°C, preferably 100 to 700°C, more preferably 300 to 700°C, and most preferably 450 to 650°C.

[0303] Embodiment 29. The method according to any one of Embodiments 22 to 28, wherein the supplied oxygen-containing gas is air, oxygen-enriched air, or oxygen gas.

[0304] Embodiment 30. The method according to any one of Embodiments 22 to 29, wherein the fuel comprises a gaseous or liquid hydrocarbon, preferably natural gas, fuel oil, or H2.

[0305] Embodiment 31. The method according to any one of Embodiments 22 to 30, wherein the oxygen-containing gas is supplied in an amount that produces an excess of oxygen relative to the amount of oxygen required for the complete combustion of the fuel, and / or the oxygen-containing gas is supplied in an amount in which 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 less than 0.7 to 1.

[0306] Embodiment 32. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material is injected through a plurality of inlets, preferably radially and perpendicularly to the central longitudinal axis of the reactor.

[0307] Embodiment 33. The method according to any one of the preceding embodiments, wherein the concentration of O2 in the high-temperature gas stream is less than 5 volume%, preferably less than 4 volume%, more preferably 0.01 to 3 volume%, and most preferably 0.1 to 2 volume%.

[0308] Embodiment 34. The method according to any one of the preceding embodiments, wherein the carbon black obtained comprises recovered carbon black and new carbon black.

[0309] Embodiment 35. The method according to any one of the preceding embodiments, wherein the residence time is the time between the injection of the particulate carbon-containing raw material into the reactor and the quenching of the resulting mixture, and is 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.

[0310] Embodiment 36. The method according to any one of the preceding embodiments, wherein the residence time of the particulate carbon-containing raw material is 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

[0311] Aspect 37. The volumetric flow rate is the volume of the fluid after injection of the particulate carbon-containing raw material in the high-temperature gas stream per unit second, and preferably, the volume of the fluid is calculated according to the ideal gas law according to Equation (2), and the method according to Aspect 36.

Number

[0312] Aspect 38. The residence time is selected such that the C, H-containing material in the particulate carbon-containing raw material is completely thermally decomposed, and the method according to any one of Aspects 35 to 37.

[0313] Aspect 39. (e) Further comprising quenching the high-temperature gas stream after injection by step (d), and the method according to any one of the preceding aspects.

[0314] Aspect 40. The high-temperature gas stream is quenched (e) 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%, still 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 according to ASTM D1618-18, and the method according to any one of the preceding aspects. [[ID=?]] [[ID=?]]

[0315] [[ID=?]] Embodiment 41. The method according to any one of the preceding embodiments, wherein the transmittance at 425 nm of the generated carbon black is measured, and the quenching position is adjusted until the transmittance at 425 nm of the generated carbon black 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.

[0316] Embodiment 42. The quenching position in the co-cooled reactor is selected such that 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, as described in any one of the preceding embodiments.

[0317] Embodiment 43. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material is 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.

[0318] Embodiment 44. The method according to any one of the preceding embodiments, wherein the reaction volume of the reactor is the volume of the reactor between the injection position of the particulate carbon-containing raw material and the quenching position.

[0319] Embodiment 45. The method according to any one of Embodiments 2 to 44, wherein deaggregation is carried out by (i) accelerating a particulate carbon-containing raw material and / or (ii) preferably by applying a shear force using an extruder.

[0320] Embodiment 46. The method according to any one of Embodiments 2 to 45, wherein deagglomeration is carried out (i) in a feed mixer, preferably including a nozzle, and / or (ii) in an extruder.

[0321] Embodiment 47. The method according to any one of Embodiments 2 to 46, wherein deagglomeration is performed in (i) a feed mixing device including a Laval nozzle.

[0322] Embodiment 48. The method according to any one of Embodiments 2 to 47, wherein deagglomeration is carried out by subjecting a particulate carbon-containing raw material to carrier gas injection.

[0323] Embodiment 49. A method according to any one of Embodiments 2 to 48, wherein deagglutination is carried out in an apparatus for supplying and mixing particles into a reactor: Here, the supply mixing device is (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, the at least one outlet having fluid communication with a deagglutination conduit, (vii) Means for accelerating and injecting a carrier gas flow into a mixing chamber.

[0324] Embodiment 50. The method according to any one of Embodiments 2 to 49, wherein the deaggregated particulate carbon-containing raw material is injected into a 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.

[0325] Embodiment 51. The method according to any one of the preceding embodiments, wherein the particulate carbon-containing raw material is contained in a carrier gas.

[0326] Embodiment 52. The method according to any one of Embodiments 2 to 51, wherein the deaggregated particulate carbon-containing raw material is contained in a carrier gas.

[0327] Embodiment 53. The method according to any one of Embodiments 2 to 52, wherein the deaggregated particulate carbon-containing raw material is contained in a carrier gas, and the carrier gas further comprises H2O and / or additives.

[0328] Embodiment 54. The method according to any one of Embodiments 2 to 53, wherein the deaggregated particulate carbon-containing raw material is contained in a carrier gas, and the carrier gas further contains H2O in an amount of 1 to 10 volume% based on the total volume of the carrier gas containing the deaggregated particulate carbon-containing raw material.

[0329] Embodiment 55. The method according to any one of the preceding embodiments, 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.

[0330] Embodiment 56. The particulate carbon-containing raw material is classified and preferably sieved before being injected into the reactor. The method according to any one of the preceding embodiments, preferably (a) the sieve having openings of 2000 μm, 1000 μm, 500 μm, 250 μm, or 125 μm, preferably 500 μm, 250 μm, or 125 μm, and / or (b) the sieve having openings of a size that captures particles having a size greater than 2000 μm, greater than 1000 μm, greater than 500 μm, greater than 250 μm, or greater than 125 μm, preferably greater than 500 μm, greater than 250 μm, or greater than 125 μm.

[0331] Embodiment 57. The method according to any one of the preceding embodiments, wherein 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 of particulate carbon-containing raw material has 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).

[0332] Embodiment 58. The method according to any one of the preceding embodiments, wherein 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 of particulate carbon-containing raw material having a particle size of less than 500 μm, the particle size being measured according to ASTM D1511-12 (2017).

[0333] Embodiment 59. The method according to any one of the preceding embodiments, wherein particulate carbon-containing raw materials 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, have a particle size of less than 1 mm, and this particle size is measured according to ASTM D1511-12 (2017).

[0334] Embodiment 60. The method according to any one of the preceding embodiments, wherein 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 of particulate carbon-containing raw material having a particle size of less than 2 mm, preferably less than 250 μm, and the particle size is measured according to ASTM D1511-12 (2017).

[0335] Embodiment 61. Carbon black manufactured according to the method of any one of the preceding embodiments, and / or (I) Carbon black with the following physical properties BET surface area is 80-90m 2 / g, and the oil absorption under compression is 58 - 69 mL / 100 g; here, the BET surface area is measured according to ASTM D6556 - 21, and the oil absorption under compression is measured using paraffin oil according to ASTM D3493 - 20; and / or (II) Carbon black having the following physical properties The BET surface area is 70 - 85 m 2 / g, and the oil absorption under compression is 59 - 70 mL / 100 g; here, the BET surface area is measured according to ASTM D6556 - 21, and the oil absorption under compression is measured using paraffin oil according to ASTM D3493 - 20; and / or (III) Carbon black having the following physical properties The BET surface area is 80 - 96 m 2 / g, and the oil absorption under compression is 60 - 69 mL / 100 g; here, the BET surface area is measured according to ASTM D6556 - 21, and the oil absorption under compression is measured using paraffin oil according to ASTM D3493 - 20; and / or (IV) Carbon black having the following physical properties The BET surface area is 120 - 138 m 2 / g, and the oil absorption under compression is 58 - 69 mL / 100 g; here, the BET surface area is measured according to ASTM D6556 - 21, and the oil absorption under compression is measured using paraffin oil according to ASTM D3493 - 20; and / or (V) Carbon black having the following physical properties The BET surface area is 82 - 95 m 2 / g, and the oil absorption under compression is 59 - 70 mL / 100 g; here, the BET surface area is measured according to ASTM D6556 - 21, and the oil absorption under compression is measured using paraffin oil according to ASTM D3493 - 20.

[0336] Aspect 61b. The carbon black according to aspect 61, wherein (I) Preferably, the BET surface area is 85 - 88 m 2The values ​​are / g, preferably the compressible oil absorption is 61-64 mL / 100g, and preferably the STSA surface area is 72-82 m². 2 The value is / g, and more preferably the STSA surface area is 76-79 m². 2 Carbon black having a density of / g, preferably with a volatile content of 2.1-2.7% by weight, more preferably with a volatile content of 2.3-2.5% by weight, preferably with a transmittance of more than 50% at 425nm in toluene, more preferably with a transmittance of more than 77% at 425nm in toluene; where the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured using paraffinic oil according to ASTM D3493-20, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (II) Preferably, the BET surface area is 77 to 79 m² 2 The values ​​are / g, preferably the compressible oil absorption is 63-65 mL / 100g, and preferably the STSA surface area is 68-78 m². 2 The value is / g, and more preferably the STSA surface area is 71-73m². 2 Carbon black having a compressible oil absorption of 58-69 mL / 100g, more preferably 63-65 mL / 100g, preferably 2.0-2.6% by weight, more preferably 2.2-2.4% by weight, preferably a transmittance of over 40% at 425 nm in toluene, more preferably over 56% at 425 nm in toluene; where the BET surface area is measured according to ASTM D6556-21, the compressible oil absorption is measured using paraffinic oil according to ASTM D3493-20, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425 nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (III) Preferably, the BET surface area is 89-92 m² 2The values ​​are / g, preferably the compressible oil absorption is 63-65 mL / 100g, and preferably the STSA surface area is 79-87 m². 2 The value is / g, and more preferably the STSA surface area is 82-84m². 2 Carbon black having a density of / g, preferably with a volatile content of 2.2-2.9% by weight, more preferably with a volatile content of 2.5-2.7% by weight, preferably with a transmittance of more than 40% at 425nm in toluene, more preferably with a transmittance of more than 62% at 425nm in toluene; where the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured using paraffinic oil according to ASTM D3493-20, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (IV) Preferably, the BET surface area is 127 to 130 m² 2 The values ​​are / g, preferably the compressible oil absorption is 62-64 mL / 100g, and preferably the STSA surface area is 82-95 m². 2 The value is / g, and more preferably the STSA surface area is 87-89 m². 2 Carbon black having a density of / g, preferably with a volatile content of 2.6-3.2% by weight, more preferably with a volatile content of 2.8-3.0% by weight, preferably with a transmittance of more than 60% at 425nm in toluene, more preferably with a transmittance of more than 80% at 425nm in toluene; where the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured according to ASTM D3493-20 using paraffinic oil, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (V) Preferably, the BET surface area is 86-89 m² 2 The values ​​are / g, preferably the compressible oil absorption is 63-65 mL / 100g, and preferably the STSA surface area is 70-82 m². 2The value is / g, and more preferably the STSA surface area is 76-78m². 2 Carbon black having a density of / g, preferably with a volatile content of 1.8-2.4% by weight, more preferably with a volatile content of 2.0-2.2% by weight, preferably with a transmittance of more than 60% at 425nm in toluene, more preferably with a transmittance of more than 80% at 425nm in toluene; where the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured according to ASTM D3493-20 using paraffinic oil, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425nm in toluene is measured relative to toluene according to ASTM D1618-18.

[0337] Appearance 62. (A) Elastomer polymer materials, and (B) Carbon black obtained according to any one of embodiments 1 to 61 and 61b, A composition containing the following:

[0338] Appearance 63. An article made from or containing the composition described in Appearance 62.

[0339] Appearance 64. Use of particulate carbon-containing raw materials for the production of carbon black in a co-flow reactor.

[0340] Embodiment 65. The use according to Embodiment 64, wherein particulate carbon-containing raw material in an amount of 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, has 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).

[0341] Embodiment 66. The residence time of the particulate carbon-containing raw material is 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), as described in any one of Embodiments 64 and 65:

number

[0342] Embodiment 67. The use according to any one of Embodiments 64 to 66, wherein a deaggregated particulate carbon-containing raw material is used.

[0343] Embodiment 68. A method for adjusting the quenching position in a co-flow reactor for producing carbon black from a particulate carbon-containing raw material, I) Injecting particulate carbon-containing raw materials into the high-temperature gas flow of a co-current reactor, where the high-temperature gas flow has a temperature of at least 800°C. II) Rapid cooling of the high-temperature gas stream containing the generated carbon black, II) Measuring the transmittance of the generated carbon black, III) Adjust the quenching position in the co-current reactor 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. A method that includes this. [Examples]

[0344] Example 1: Rubber granules

[0345] 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.

[0346] 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. However, the present invention is not limited to the feed mixer shown in Figure 1, as other feed mixers can be used. The rubber granules used in the experiment, i.e., rubber granules 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.

[0347] [Table 1]

[0348] Table 2 shows the properties of rubber granules from ESTATO.

[0349] [Table 2]

[0350] Furthermore, the rubber granules contain several metals at a mass fraction of approximately 300 ppm, such as zinc and iron.

[0351] 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

[0352] 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.

[0353] 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.

[0354] The daily coefficient is calculated as follows:

number

[0355] 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.

[0356] 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.

[0357] 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.

[0358] 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.

[0359] Elemental concentrations are calculated according to the following formula.

number

[0360] 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.

[0361] The blank measurement is calculated as follows:

number

[0362] 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.

[0363] The daily coefficient is calculated as follows:

number

[0364] 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. The samples are then measured.

[0365] Elemental concentrations are calculated according to the following formula.

number

[0366] Reaction conditions in a furnace reactor

[0367] 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.

[0368] [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.

[0369] [Table 4]

[0370] 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.

[0371] 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.

[0372] 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.

[0373] The carbon black obtained in each experiment was characterized, and the results are shown in Table 4.

[0374] [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. 6The 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. 12 The 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.

[0375] [Table 6]

[0376] 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”.

[0377] 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.

[0378] 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

[0379] 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.

[0380] 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.

[0381] 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.

[0382] Example 2: Rubber composition

[0383] 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.

[0384] 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.

[0385] Next, during the second final mixing step, sulfur and accelerator (Vulkacit CZ / EG-Z) were added in the indicated amounts to the masterbatch obtained from the first mixing step. The resulting mixture was ground in a GK1.5E mixer for 2 minutes at a chamber temperature of 40°C and a packing density of 0.64. The rotor speed was 30 rpm, and the batch temperature was kept below 110°C. Finally, the mixture was removed from the internal mixer and processed again in an open mill. The resulting vulcanizable composition (green compound) was cured at a temperature of 165°C for 11–15 minutes (C1: 15 min, C2: 12 min, C3: 12 min, C4: 12 min, C5: 11 min, C6: 12 min, C7: 12 min, C8: 11 min, C9: 11 min).

[0386] [Table 7] 16 Rubber ESBR, Buna SB1500, Reginex Germany 17 Carbon black: N660, N550, rCB, or Experiments A3-5 and A8-A10 (see Table 6) 18 6PPD, VULKANOX4020 / LG, Brentag 19 Sulfur, MAHLSCHWEFEL80 / 90°, oil-free, Avocal 20 CBS, VULKACIT CZ / EG-C, LANXESS 21 ZnO, ZNO RS RAL844C, Norchem 22 Stearic acid, Palmera B1804, Calbic Germany

[0387] The properties of the test specimens were measured, and the results are shown in Table 6. The results are compared with those of carbon black produced using liquid carbon black raw materials (N660 and N550) and recovered carbon black rCB.

[0388] [Table 8] 23 The loss factor tan(d) was measured as described below. 24 The relative peak area of ​​the topography was measured as described below. 25 Tensile strength was measured according to ISO 37-2012, S2. 26 Elongation at fracture was measured according to ISO 37-2012, S2. 27 Wear was measured at 23°C, DIN ISO4649:2014-03, 10N. 28 The elastic modulus of 300% was measured according to ISO 37-2012, S2. 29 Ball rebound was measured at 60°C according to ASTM D2632:2015. 30 Tear resistance was measured using DIN ISO34-1:2016-09, Method B, mutant (b). [Table 9]

[0389] Relative peak area of ​​topography

[0390] The relative peak area of ​​topography is an indicator of filler dispersion determined by surface topography (including medallion correction), following the procedure described in A. Wehmeyer, "Analysis of Filler Dispersion by Topographic Measurement," Technical Report TR820, Degussa, and A. Wehmeyer, "Development of a Characterization Method for Filler Dispersion in Rubber Mixtures Using Surface Topography," Master's Thesis, 1998, Münster University of Applied Sciences, and DE19917975C2.

[0391] Loss factor tan(d) The above values ​​and the loss coefficient tan(d) were measured according to DIN53 513, using a cylindrical specimen (height 10 mm, diameter 10 mm) in strain control mode (1 ± 0.5 mm) or force control mode (50 N ± 25 N), at 60°C and a frequency of 16 Hz.

[0392] 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.

[0393] 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]

[0394] 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 method for producing carbon black from a particulate carbon-containing raw material in a co-flow reactor having a flow channel along the central longitudinal axis of the reactor, (a) To provide a high-temperature gas flow, (b) To provide a raw material containing particulate carbon, (d) The process includes injecting particulate carbon-containing raw materials into a high-temperature gas stream to form carbon black, A method wherein the high-temperature gas flow has a temperature of at least 800°C.

2. The method according to claim 2, wherein the particulate carbon-containing raw material includes rubber granules, plastic granules, and / or biomass-based granules, preferably the particulate carbon-containing raw material includes rubber granules, and the rubber granules include carbon black.

3. The method according to claim 1 or 2, wherein 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 of particulate carbon-containing raw material has 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 the particle size is measured according to ASTM D1511-12 (2017).

4. A method according to any one of claims 1 to 3, wherein the particle size distribution of the particulate carbon-containing raw material is measured according to ASTM D1511-12 (2017), (a) Sieve number 10 holds 1 to 0 to 10% by weight, preferably 1 to 8% by weight, more preferably 1 to 5% by weight, 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, and / or 5 to 12% by weight of 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, and most preferably 25 to 55% by weight of particulate carbon-containing raw material, and / or (d) Sieve number 60 holds 5 to 70% by weight, preferably 10 to 60% by weight, more preferably 15 to 50% by weight, and most preferably 20 to 45% by weight of particulate carbon-containing raw material, and / or (e) Sieve number 120 holds 1 to 80% by weight, preferably 7 to 70% by weight, more preferably 5 to 60% by weight, and / or (f) A method wherein the bottom tray contains particulate carbon-containing raw material in an amount of less than 4% by weight, preferably less than 3% by weight, more preferably 0 to 2% by weight, and most preferably 0.01 to 1% by weight.

5. The method according to any one of claims 1 to 4, wherein the high-temperature gas flow is obtained by electric preheating, plasma heating, and combustion of a fuel and oxygen-containing gas, and / or the co-flow reactor is a furnace reactor.

6. Before being injected into the reactor, the particulate carbon-containing raw material is classified and preferably sieved. The method according to any one of claims 1 to 5, preferably (a) the sieve having an opening of 2000 μm, 1000 μm, 500 μm, 250 μm, or 125 μm, preferably 500 μm, 250 μm, or 125 μm, and / or (b) the sieve having an opening of a size that captures particles having a size greater than 2000 μm, greater than 1000 μm, greater than 500 μm, greater than 250 μm, or greater than 125 μm, preferably greater than 500 μm, greater than 250 μm, or greater than 125 μm.

7. The residence time of the particulate carbon-containing raw material is 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), according to any one of claims 1 to 6: [Math 1] In the formula, t ｒ V is the residence time, and V is the volume of the reaction (m³). ３ ) and Q is the volumetric flow rate (m ３ *s －１ )

8. The method according to any one of claims 1 to 7, wherein the quenching position in the co-cooled reactor is selected such that 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.

9. The method according to any one of claims 1 to 8, wherein the particulate carbon-containing raw material is injected into the reactor at a mass flow rate of 2 to 50 kg / h per 130 L of the reactor's reaction volume, preferably 5 to 40 kg / h per 130 L of the reactor's reaction volume, more preferably 8 to 30 kg / h per 130 L of the reactor's reaction volume, and most preferably 10 to 20 kg / h per 130 L of the reactor's reaction volume.

10. The method according to any one of claims 1 to 9, wherein step (b) further comprises deaggregating a particulate carbon-containing material, and in step (d), the deaggregated particulate carbon-containing material is injected into a high-temperature gas stream to form carbon black, and the deaggregation is carried out by (i) accelerating the particulate carbon-containing material and / or (ii) preferably by applying a shear force using an extruder.

11. Carbon black produced by the method described in any one of claims 1 to 10, and / or (I) Carbon black with the following physical properties BET surface area is 80-90 m² ２ The value is / g, and preferably the BET surface area is 85 to 88 m². ２ / g, The compressed oil absorption capacity is 58 to 69 mL / 100g, preferably 61 to 64 mL / 100g. Preferably, the STSA surface area is 72 to 82 m². ２ The value is / g, and more preferably the STSA surface area is 76 to 79 m². ２ / g, Preferably, the volatile content is 2.1 to 2.7% by weight, and more preferably, the volatile content is 2.3 to 2.5% by weight. Preferably, the transmittance at 425 nm in toluene is greater than 50%, and more preferably, the transmittance at 425 nm in toluene is greater than 77%; Here, the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured using paraffinic oil according to ASTM D3493-20, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425 nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (II) Carbon black with the following physical properties The BET specific surface area is 70 to 85 m ２ / g, preferably the BET specific surface area is 77 to 79 m ２ / g, and The compressed oil absorption capacity is 59 to 70 mL / 100 g, preferably 63 to 65 mL / 100 g. Preferably, the STSA surface area is 68 to 78 m². ２ The value is / g, and more preferably the STSA surface area is 71 to 73 m². ２ / g, Preferably, the compressible oil absorption capacity is 58 to 69 mL / 100g, and more preferably, the compressible oil absorption capacity is 63 to 65 mL / 100g. Preferably, the volatile content is 2.0 to 2.6% by weight, and more preferably, the volatile content is 2.2 to 2.4% by weight. Preferably, the transmittance at 425 nm in toluene is greater than 40%, and more preferably, the transmittance at 425 nm in toluene is greater than 56%; Here, the BET surface area is measured according to ASTM D6556-21, the compressed oil absorption is measured using paraffinic oil according to ASTM D3493-20, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425 nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (III) Carbon black with the following physical properties BET surface area of ​​80-96 m² ２ The value is / g, and preferably the BET surface area is 89 to 92 m². ２ / g, The compressed oil absorption capacity is 60 to 69 mL / 100 g, preferably 63 to 65 mL / 100 g. Preferably, the STSA surface area is 79 to 87 m². ２ The value is / g, and more preferably the STSA surface area is 82 to 84 m². ２ / g, Preferably, the volatile content is 2.2 to 2.9% by weight, and more preferably, the volatile content is 2.5 to 2.7% by weight. Preferably, the transmittance at 425 nm in toluene is greater than 40%, and more preferably, the transmittance at 425 nm in toluene is greater than 62%; Here, the BET surface area is measured according to ASTM D6556-21, the compression oil absorption is measured using paraffinic oil according to ASTM D3493-20, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425 nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (IV) Carbon black with the following physical properties BET surface area of ​​120-138 m² ２ The value is / g, and preferably the BET surface area is 127 to 130 m². ２ / g, The compressed oil absorption capacity is 58 to 69 mL / 100g, preferably 62 to 64 mL / 100g. Preferably, the STSA surface area is 82 to 95 m². ２ The value is / g, and more preferably the STSA surface area is 87 to 89 m². ２ / g, Preferably, the volatile content is 2.6 to 3.2% by weight, and more preferably, the volatile content is 2.8 to 3.0% by weight. Preferably, the transmittance at 425 nm in toluene is greater than 60%, and more preferably, the transmittance at 425 nm in toluene is greater than 80%; Here, the BET surface area is measured according to ASTM D6556-21, the compressible oil absorption is measured according to ASTM D3493-20 using paraffinic oil, the STSA surface area is measured according to ASTM D6556-21, the volatile content is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425 nm in toluene is measured relative to toluene according to ASTM D1618-18; and / or (V) Carbon black with the following physical properties BET surface area is 82-95 m² ２ The value is / g, and preferably the BET surface area is 86 to 89 m². ２ / g, The compressed oil absorption capacity is 59 to 70 mL / 100 g, preferably 63 to 65 mL / 100 g. Preferably, the STSA surface area is 70 to 82 m². ２ The value is / g, and more preferably the STSA surface area is 76 to 78 m². ２ / g, Preferably, the volatile content is 1.8 to 2.4% by weight, and more preferably, the volatile content is 2.0 to 2.2% by weight. Preferably, the transmittance at 425 nm in toluene is greater than 60%, and more preferably, the transmittance at 425 nm in toluene is greater than 80%; Here, the BET surface area is measured according to ASTM D6556-21, the compressible oil absorption is measured according to ASTM D3493-20 using paraffinic oil, the STSA surface area is measured according to ASTM D6556-21, the volatile matter is measured at 950°C for 7 minutes as described in the specification, and the transmittance at 425 nm in toluene is measured relative to toluene according to ASTM D1618-18.

12. (A) Elastomer polymer materials, and (B) Carbon black obtained according to any one of claims 1 to 10, A composition containing the following:

13. An article made from or containing the composition described in claim 12.

14. Use of particulate carbon-containing raw materials for carbon black production in a co-flow reactor.

15. A method for adjusting the quenching position in a co-flow reactor for producing carbon black from a particulate carbon-containing raw material, I) Injecting particulate carbon-containing raw materials into the high-temperature gas flow of a co-current reactor, where the high-temperature gas flow has a temperature of at least 800°C. II) Rapid cooling of the high-temperature gas stream containing the generated carbon black, II) Measuring the transmittance of the generated carbon black, III) Adjust the quenching position in the co-flow reactor 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. A method that includes this.

Images