EP0639631B1 - Verfahren zur Herstellung von Synthesegas - Google Patents

Verfahren zur Herstellung von Synthesegas Download PDF

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Publication number
EP0639631B1
EP0639631B1 EP94112796A EP94112796A EP0639631B1 EP 0639631 B1 EP0639631 B1 EP 0639631B1 EP 94112796 A EP94112796 A EP 94112796A EP 94112796 A EP94112796 A EP 94112796A EP 0639631 B1 EP0639631 B1 EP 0639631B1
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EP
European Patent Office
Prior art keywords
liquid
products
cracking
gas
carried out
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
Application number
EP94112796A
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German (de)
English (en)
French (fr)
Other versions
EP0639631A1 (de
Inventor
Ulrich Gerhardus
Horst Dr. Hanke
Josef Hibbel
Norbert Leder
Klaus Poloszyk
Heinz Scheve
Volkmar Schmidt
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Celanese Sales Germany GmbH
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Celanese GmbH
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Publication date
Application filed by Celanese GmbH filed Critical Celanese GmbH
Publication of EP0639631A1 publication Critical patent/EP0639631A1/de
Application granted granted Critical
Publication of EP0639631B1 publication Critical patent/EP0639631B1/de
Anticipated expiration legal-status Critical
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G1/00—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal
    • C10G1/10—Production of liquid hydrocarbon mixtures from oil-shale, oil-sand, or non-melting solid carbonaceous or similar materials, e.g. wood, coal from rubber or rubber waste
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels

Definitions

  • the invention relates to a method for converting Plastic waste in synthesis gas that is used as a raw material for chemical syntheses can be used.
  • Plastic waste can only be burned without special precautions should be discarded if it is ensured that no pollutants in the Environment. This requirement is only in exceptional cases given, because they often contain chlorine, but also components containing sulfur or nitrogen as well as heavy metals that are undesirable during combustion Products of combustion. Dedusting and Flue gas scrubbing, if necessary special combustion devices, are then indispensable. Delivery and dosage problems can also occur if the Waste non-combustible and non-melting foreign substances contains. Furthermore, economic reasons argue against high-quality finishing products of petrochemical raw materials like their raw materials, namely petroleum and petroleum products, to burn.
  • Waste from plastic and rubber are being re-used the process described in DE-C-2 205 001 thermally at 250 to 450 ° C in the presence of one at the reaction temperature split liquid auxiliary phase. Arise over 90% liquid hydrocarbons and only in subordinate ones Amounts of soot.
  • thermal processing One of the primary goals of thermal processing is the conversion of plastics into liquid fuels, which are easily conveyed and dosed and in the combustion air can be distributed homogeneously to a smoke and ensure soot-free combustion.
  • hydrocarbons e.g. as a solution, Extraction or cleaning agents are not excluded.
  • a major disadvantage of the known methods is the need to comply with the plastics Temperatures and dwell times very largely dismantle. Furthermore, they require an expensive one Separation of those often contained in the plastics Solids such as inorganic or organic pigments, Opacifiers and fillers.
  • the invention has for its object plastic waste to convert into technically usable raw materials.
  • solids are incorporated into the plastics concentrated and free of organic components accumulate, so that they are environmentally friendly can be disposed of.
  • This object is achieved by a manufacturing method of synthesis gas from plastic waste. It is characterized in that the waste thermally predominantly split into liquid products and the liquid Fission products due to partial oxidation in synthesis gas be transferred.
  • plastic waste in the sense of the new process is very broad. It closes uniform Substances and mixtures of substances of whatever origin and Composition a. According to their thermal behavior the wastes are derived from thermoplastic or thermoset Plastics.
  • plastic waste include used plastics for packaging purposes served or as materials, e.g. in construction, electrical or textile industry, in machine and vehicle construction, have been used or for everyday items, processed like household and sports equipment or toys had been.
  • Plastic waste is also bad batches and residues and residues from production and Processing. Plastic waste can therefore be short Designate plastic material that does not regenerate or another economic exploitation leaves. Waste can be processed using the new process e.g.
  • plastics polyolefins, Vinyl resins such as polyvinyl chloride, polyvinyl acetate and Polyvinyl alcohol, also polystyrenes, polycarbonates, Polymethylene oxides, polyacrylates, polyurethanes, polyamides, Polyester resins as well as hardened epoxy resins.
  • polyolefins Vinyl resins such as polyvinyl chloride, polyvinyl acetate and Polyvinyl alcohol, also polystyrenes, polycarbonates, Polymethylene oxides, polyacrylates, polyurethanes, polyamides, Polyester resins as well as hardened epoxy resins.
  • Vinyl resins such as polyvinyl chloride, polyvinyl acetate and Polyvinyl alcohol
  • polystyrenes polycarbonates
  • Polymethylene oxides Polyacrylates
  • polyurethanes polyamides
  • Polyester resins as well as hardened epoxy resins.
  • thermoplastic is simple Perform plastics.
  • the feed material from which is rough Impurities such as metals, glass and ceramic materials were mechanically separated, thermally to low molecular weight Dismantled fragments.
  • Impurities such as metals, glass and ceramic materials
  • the cleavage of the polymeric compounds can in In the presence or absence of hydrogen. There is also a subsequent hydrogenation of the cleavage products possible; however, it is not the sub-step thermal pretreatment of the waste is absolutely necessary, to work under hydrating conditions. The Choosing the most suitable for the thermal degradation of plastics The process therefore largely depends on the particular Circumstances.
  • plastic waste does not only result to easily dosed and homogeneous, liquid products.
  • it also has a dechlorination in the Plastic waste, which often contains chlorine Plastics.
  • the halogen is called Hydrogen chloride split off from the gaseous Degradation products are washed out in a known manner.
  • the Liquid fission products only contain chlorine in small amounts Quantities tolerable in the subsequent gasification are.
  • Thermal treatment has proven to be particularly suitable of plastic waste at temperatures between 250 and 450 ° C using one at the reaction temperature proven liquid auxiliary phase (see. DE-C-2 205 001).
  • This auxiliary phase is used in particular to transfer the Heat on the feed materials in the cracking reactor. About that it also promotes thermal degradation in that it in many cases the starting materials swell like a gel leaves.
  • Such substances are successfully used as an auxiliary phase applied, the waste products used and the Fission products at the given reaction temperature at least partially solve. Natural have proven themselves or artificial waxy hydrocarbons, further Polyglycols and especially the liquid degradation products the plastic waste itself.
  • the dismantling of the waste to be processed is promoted by that you mechanically before thermal splitting crushed. In addition, he can add more suitable Catalysts are accelerated. So you can Waste containing mainly polyolefins in the presence of manganese, vanadium, copper, chrome, molybdenum or tungsten compounds easily at elevated temperature split into small molecules.
  • the catalytic Effective metals can already be found in plastics are in the form of additives, so that their addition is unnecessary.
  • the high-molecular feedstocks are converted in conventional reactors, e.g. in closed, with a stirring kettle provided. Usually you work in one step. Especially when develop aggressive gases when processing waste, it is recommended that the splitting process two or to carry out in several stages, the split in the individual Stages generally not at the same temperature, but with increasing temperatures from level to level is operated. This is how it is with chlorine containing polymer proved to be useful, water-moist Plastics first at moderate temperature, the not yet leading to the HCl elimination, to dry one corrosive stress on the reactor materials to avoid aqueous hydrogen chloride. Only after the Drying, the temperature is increased so far that as a result of the cleavage of the polymers hydrogen chloride forms.
  • the dechlorination can be done in an additional Level by further increasing the temperature and the dwell time are completed.
  • the gradually Thermal degradation of chlorine-containing polymeric substances allows, by choosing the reaction temperature, the fission products producing aggressive gases preferred in to enrich the first gap stage, so that in the subsequent Separation of gases harmful to the environment only part of the fission products of a cleaning device must be fed.
  • the chlorine on a scale of about 5 wt .-%, according to the invention Process converted into liquid fission products whose chlorine content is only a few 100 ppm is.
  • the fission products boil in the area of raw gasoline (Naphtha) and the middle distillates and also own the Viscosity of these petroleum fractions. You can therefore be pump with conventional devices.
  • hydrocarbons formed during the splitting the reactor partly as vapors mixed with Hydrogen chloride and small amounts of other fission gases like carbon monoxide, hydrogen, nitrogen and ammonia. They are made from the gaseous mixture by partial Condensation obtained as an ash-free condensate. It is one for further processing, e.g. on naphtha, suitable raw material.
  • the gas phase containing hydrogen chloride can e.g. be converted into about 30% hydrochloric acid.
  • the remaining part of the fission product which is the total Ash contains, is discharged liquid and alone or mixed with other raw materials, e.g. Naphtha, with Water vapor and oxygen converted to synthesis gas.
  • a process that is particularly relevant to pollutant avoidance the claims outlined above is sufficient, e.g. in EP-A-0 515 950. It is characterized in that the feed oxidized under conditions that lead to the formation of about 0.1 up to about 0.3% by weight of carbon black, based on the in the form of Carbon used hydrocarbons. This way of working can also be successfully applied to the Conversion of waste products from plastic waste into Use carbon monoxide-hydrogen mixtures. In this Case is the carbon content of the depolymerized Plastics reference value for the soot content. Its height is in a known manner about the amount of oxygen supplied set, moreover, the use recommend a specially designed burner (see e.g. EP-B-0 095 103).
  • the gasification itself takes place at temperatures between 1100 and 1500 ° C and a pressure of 1 up to 10 MPa. That the gasification reactor with a temperature from 1300 to 1500 ° C leaving raw gas contains in addition Soot in the specified amount of metals and / or metal compounds in liquid form. It will initially be in one Radiation cooler pre-cooled to 500 to 1000 ° C, one temperature range, in which the metallic contaminants solidify without substantial contact with the cooler wall. Some of the solid particles settle in the water sump of the radiation cooler and are discharged from there. For further cooling to 150 to 300 ° C, preferably 260 to 280 ° C, you can manage the rest Portions of fine metal particles and soot particles Raw gas in a convection cooler.
  • the carbon monoxide / hydrogen mixture obtained by gasifying the depolymerized plastic waste can be used directly as a starting material for chemical reactions, for example for oxosynthesis.
  • the C / H ratio of their fission products is lower than that of heavy fuel oils, the common raw material for synthesis gas production.
  • the CO / H 2 ratio of 1: 1 required for certain applications (eg in the oxo process) is therefore not always achieved.
  • a hydrogen-rich fraction can be separated from the solid-free raw gas in a membrane system, which is burned or worked up by conversion to pure hydrogen.
  • the gas mixture as a whole can also be converted into hydrogen by conversion.
  • the figure shows the new process in the form of a block diagram.
  • Plastic waste is broken down thermally in the depolymerization stage at temperatures which, depending on the process, are in the range of 200 to 500 ° C to liquid products, the flowability of which corresponds roughly to that of heavy heating oils at the same temperature.
  • the depolymerization is accompanied by the splitting off of hydrogen chloride from chlorine-containing plastics, the hydrogen chloride is washed out with water from the reaction product and worked up in a known manner, for example to 30% crude acid. In special cases, the hydrogen chloride can also be neutralized in an alkaline wash.
  • the splitting is followed by gasification, ie the partial oxidation of the depolymerized waste with oxygen in the presence of water vapor.
  • Chlorine-carbon compounds remaining in low concentrations in the cleavage product do not impair this process step.
  • the CO / H 2 mixture resulting from the gasification is washed to remove solids and HCl with water, to which alkaline reagents such as alkali metal carbonate or hydroxide have optionally been added.
  • alkaline reagents such as alkali metal carbonate or hydroxide have optionally been added.
  • the raw gas is passed through a membrane filter.
  • hydrogen can also be obtained from the raw gas.
  • it is converted, the resulting CO 2 / H 2 mixture is sent to a chemical wash and separated into CO 2 and H 2 in a pressure swing absorption stage.
  • Recycled packaging material made of plastic with a content of 2.5% by weight of water and 3.3% by weight of chlorine is suspended in a liquid auxiliary phase, which was obtained by thermal splitting of plastic waste, and to separate the water at about 130 ° C. heated.
  • the plastic suspension is then transferred to the cleavage reactor, in which the feed material is depolymerized at about 350 ° C. and has a residence time of about 4 hours. Gaseous fission products are cooled to about 30 ° C and fed to an appropriate absorption system for the separation of hydrogen chloride.
  • Part of the liquid fission product is used as an auxiliary phase (suspension medium) for the thermal fission of further plastic waste, the rest is partially oxidized to water gas.
  • the depolymerizate is reacted with oxygen and water vapor in a known manner at about 1400 ° C. and a pressure of 4 MPa.
  • 400 kg depolymerizate 325 Nm 3 oxygen and 110 kg steam are required.
  • the raw gas contains 43.8 vol% CO, 48.6 vol% H 2 and 6.6 vol% CO 2 ; the CO / H 2 ratio is about 0.9.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Wood Science & Technology (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Separation, Recovery Or Treatment Of Waste Materials Containing Plastics (AREA)
  • Processing Of Solid Wastes (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Catalysts (AREA)
  • Manufacture Of Porous Articles, And Recovery And Treatment Of Waste Products (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
EP94112796A 1993-08-21 1994-08-17 Verfahren zur Herstellung von Synthesegas Expired - Lifetime EP0639631B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE4328188A DE4328188C2 (de) 1993-08-21 1993-08-21 Verfahren zur Herstellung von Synthesegas
DE4328188 1993-08-21

Publications (2)

Publication Number Publication Date
EP0639631A1 EP0639631A1 (de) 1995-02-22
EP0639631B1 true EP0639631B1 (de) 1999-11-24

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Application Number Title Priority Date Filing Date
EP94112796A Expired - Lifetime EP0639631B1 (de) 1993-08-21 1994-08-17 Verfahren zur Herstellung von Synthesegas

Country Status (10)

Country Link
US (1) US5457250A (enrdf_load_stackoverflow)
EP (1) EP0639631B1 (enrdf_load_stackoverflow)
JP (1) JP2534461B2 (enrdf_load_stackoverflow)
KR (1) KR100308464B1 (enrdf_load_stackoverflow)
AT (1) ATE186940T1 (enrdf_load_stackoverflow)
BR (1) BR9403282A (enrdf_load_stackoverflow)
CA (1) CA2130019C (enrdf_load_stackoverflow)
DE (2) DE4328188C2 (enrdf_load_stackoverflow)
ES (1) ES2141788T3 (enrdf_load_stackoverflow)
TW (1) TW310333B (enrdf_load_stackoverflow)

Families Citing this family (23)

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DE19534448A1 (de) * 1995-09-16 1997-03-20 Buna Sow Leuna Olefinverb Gmbh Verfahren zum Entsorgen von PVC, vorzugsweise zur Gewinnung von gereinigtem und/oder reinem Chlorwasserstoff
ES2198000T3 (es) * 1996-07-17 2004-01-16 Texaco Development Corporation Oxidacion parcial de material plastico residual.
AU3459500A (en) * 1999-04-02 2000-10-23 Ebara Corporation Method and apparatus for production of hydrogen by gasification of combusible material
DE19952755B4 (de) * 1999-11-02 2006-11-23 Future Energy Gmbh Verfahren und Flugstromvergaser zur Umwandlung von fließfähigen halogen- und kohlenstoffhaltigen Rest- und Abfallstoffen
DE10065921A1 (de) 1999-11-06 2001-07-26 Krc Umwelttechnik Gmbh Verfahren und Vorrichtung zur Vergasung von Brenn-, Rest- und Abfallstoffen mit Vorverdampfung
DE19954188A1 (de) 1999-11-11 2001-05-31 Krc Umwelttechnik Gmbh Verfahren und Vorrichtung zur Verwertung stickstofforganischer Verbindungen durch Vergasung
DE19957696C1 (de) 1999-11-30 2001-05-03 Krc Umwelttechnik Gmbh Vorrichtung zur Vergasung kohlenstoffhaltiger Brenn-, Rest- und Abfallstoffe in einem Flugstromreaktor
US20030192251A1 (en) * 2002-04-12 2003-10-16 Edlund David J. Steam reforming fuel processor
CN1304355C (zh) * 2004-04-08 2007-03-14 浙江大学 一种液相催化降解聚苯乙烯废旧塑料生产苯甲酸的方法
DE102009007880A1 (de) 2009-02-06 2010-08-12 Eta Ag Engineering Verfahren und Vorrichtung zur Behandlung von chlorhaltigem Rohgas aus Vergasungsanlagen
EP2417226A4 (en) * 2009-04-06 2013-08-28 Rentech Inc SYSTEM AND METHOD FOR CONDITIONING SYNTHESIS GAS DERIVED FROM BIOMASS
SG2013081963A (en) * 2013-06-04 2015-12-30 Enviro Power Pte Ltd System and method for converting plastic/rubber to hydrocarbon fuel by thermo-catalytic process
US11447576B2 (en) 2019-02-04 2022-09-20 Eastman Chemical Company Cellulose ester compositions derived from recycled plastic content syngas
US11286436B2 (en) 2019-02-04 2022-03-29 Eastman Chemical Company Feed location for gasification of plastics and solid fossil fuels
CN115052729A (zh) 2020-02-10 2022-09-13 伊士曼化工公司 废塑料密度分离
EP4136198A4 (en) * 2020-04-13 2024-08-14 Eastman Chemical Company GASIFICATION OF LIQUEFIED PLASTIC WASTE
EP4136152A1 (en) * 2020-04-13 2023-02-22 Eastman Chemical Company Chemical recycling of plastic dry fines
EP4136161A1 (en) * 2020-04-13 2023-02-22 Eastman Chemical Company Chemical recycling of plastic purge materials
WO2021211521A1 (en) * 2020-04-13 2021-10-21 Eastman Chemical Company Partial oxidation gasification of wet waste plastic
EP4136157A1 (en) * 2020-04-13 2023-02-22 Eastman Chemical Company Chemical recycling of metal-containing plastics mixtures
JP2024547219A (ja) * 2021-12-20 2024-12-26 カンツラー、ヴァルター 反応装置
KR20240138616A (ko) 2023-03-09 2024-09-20 에스케이이노베이션 주식회사 합성가스 제조방법, 제조장치 및 이를 이용한 액상 탄화수소 제조방법
WO2025143147A1 (ja) * 2023-12-28 2025-07-03 国立大学法人弘前大学 リサイクル用残留物の製造方法

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Also Published As

Publication number Publication date
US5457250A (en) 1995-10-10
JP2534461B2 (ja) 1996-09-18
DE59408948D1 (de) 1999-12-30
DE4328188A1 (de) 1995-02-23
JPH07197041A (ja) 1995-08-01
KR100308464B1 (ko) 2001-12-01
TW310333B (enrdf_load_stackoverflow) 1997-07-11
DE4328188C2 (de) 1996-04-18
ATE186940T1 (de) 1999-12-15
BR9403282A (pt) 1995-04-11
ES2141788T3 (es) 2000-04-01
KR950005959A (ko) 1995-03-20
EP0639631A1 (de) 1995-02-22
CA2130019A1 (en) 1995-02-22
CA2130019C (en) 1999-10-19

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