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EP0639631A1 - Procédé de préparation de gaz de synthèse - Google Patents

Procédé de préparation de gaz de synthèse Download PDF

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Publication number
EP0639631A1
EP0639631A1 EP94112796A EP94112796A EP0639631A1 EP 0639631 A1 EP0639631 A1 EP 0639631A1 EP 94112796 A EP94112796 A EP 94112796A EP 94112796 A EP94112796 A EP 94112796A EP 0639631 A1 EP0639631 A1 EP 0639631A1
Authority
EP
European Patent Office
Prior art keywords
liquid
products
waste
gas
plastic waste
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.)
Granted
Application number
EP94112796A
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German (de)
English (en)
Other versions
EP0639631B1 (fr
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
Original Assignee
Hoechst AG
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Filing date
Publication date
Application filed by Hoechst AG filed Critical Hoechst AG
Publication of EP0639631A1 publication Critical patent/EP0639631A1/fr
Application granted granted Critical
Publication of EP0639631B1 publication Critical patent/EP0639631B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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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 process for converting plastic waste into synthesis gas, which can be used as a raw material for chemical synthesis.
  • Plastic waste can only be disposed of by incineration without special precautionary measures if it is ensured that no pollutants are released into the environment. This requirement is only given in exceptional cases, because they often contain chlorine-containing, but also sulfur- or nitrogen-containing components, as well as heavy metals, which lead to undesired combustion products during combustion. Dust removal and flue gas scrubbing, if necessary special combustion devices, are then indispensable. Conveying and dosing problems can also occur if the waste contains non-flammable and non-melting foreign substances. In addition, economic reasons speak against burning high-quality finishing products of petrochemical raw materials such as their raw materials, namely petroleum and petroleum products.
  • a gasoline-kerosene mixture is obtained by degrading polyethylene at 400 to 450 ° C (CA Vol. 76, 1972, 158024 q). This process can also be carried out in the presence of nickel catalysts (Chem. Ind. XXIII, 1971, 630).
  • the splitting of carbon-containing organic waste Synthetic or predominantly synthetic origin takes place according to the process of EP-A-291 698 under hydrogenating conditions and results predominantly in hydrocarbon fractions in the gasoline and medium oil (diesel oil) boiling range.
  • Waste from plastic and rubber are split thermally at 250 to 450 ° C in the presence of an auxiliary phase which is liquid at the reaction temperature by the process described in DE-C-2 205 001. Over 90% liquid hydrocarbons are formed and soot is only produced in minor amounts.
  • a primary goal of thermal processing is the conversion of plastics into liquid fuels that can be easily conveyed and dosed and distributed homogeneously in the combustion air to ensure smoke-free and soot-free combustion.
  • Prior use of the hydrocarbons e.g. as a solvent, extraction or cleaning agent is not excluded.
  • a decisive disadvantage of the known methods is the need to degrade the plastics to a large extent while maintaining the appropriate temperatures and residence times.
  • they require a complex separation of the solids often contained in the plastics, such as inorganic or organic pigments, opacifiers and fillers.
  • the invention has for its object to convert plastic waste into technically usable raw materials.
  • solids incorporated into the plastics are to be concentrated in the preparation process and are free of organic constituents, so that they can be disposed of in an environmentally friendly manner.
  • This object is achieved by a process for producing synthesis gas from plastic waste. It is characterized in that the waste is thermally split predominantly into liquid products and the liquid split products are converted into synthesis gas by partial oxidation.
  • plastic waste in the sense of the new process is very broad. It includes uniform substances and mixtures of substances of whatever origin and composition.
  • the waste is derived from thermoplastic or thermosetting plastics based on their thermal behavior.
  • the plastic waste includes used plastics that were used for packaging purposes or as materials, e.g. in the construction, electrical or textile industry, in machine and vehicle construction, or were processed into articles for everyday use, such as household and sports equipment or toys.
  • Plastic waste is also faulty batches and unusable residues and residues from production and processing. Plastic waste can therefore briefly be called plastic material that cannot be regenerated or used for other economic purposes. According to the new procedure, waste e.g.
  • plastics polyolefins, vinyl resins such as polyvinyl chloride, polyvinyl acetate and polyvinyl alcohol, furthermore polystyrenes, polycarbonates, polymethylene oxides, polyacrylates, polyurethanes, polyamides, polyester resins and hardened epoxy resins.
  • the process is particularly easy to carry out with thermoplastics.
  • the feed material from which coarse impurities such as metals, glass and ceramic materials have been mechanically separated, becomes thermally low molecular weight Dismantled fragments.
  • all known processes are suitable for this process step, which preferably result in liquid decomposition products and / or soot only in a minor amount.
  • the polymeric compounds can be cleaved in the presence or absence of hydrogen. Subsequent hydrogenation of the cleavage products is also possible; However, it is not absolutely necessary in any sub-step of the thermal pretreatment of the waste to work under hydrogenating conditions. The choice of the process suitable for the thermal degradation of the plastics therefore largely depends on the respective circumstances.
  • the depolymerization of plastic waste not only leads to easily metered and homogeneous, liquid products. In particular, it also results in dechlorination of the chlorine-containing plastics that are often present in the plastic waste.
  • the halogen is split off as hydrogen chloride, which is washed out from the gaseous degradation products in a known manner.
  • the liquid fission products only contain chlorine in small amounts that can be tolerated in the subsequent gasification.
  • auxiliary phase which is liquid at the reaction temperature has proven to be particularly suitable (cf. DE-C-2 205 001).
  • This auxiliary phase is used in particular to transfer the heat to the feed materials in the cracking reactor. In addition, it promotes thermal degradation by allowing the starting materials to swell in a gel-like manner in many cases.
  • auxiliary phase such substances are used with success that the waste products used and the Dissolve cleavage products at least partially at the given reaction temperature. Natural or artificial waxy hydrocarbons, polyglycols and in particular the liquid degradation products of the plastic waste itself have proven successful.
  • the breakdown of the waste to be processed is promoted by mechanically crushing it before thermal decomposition. In addition, it can be accelerated by adding suitable catalysts. In this way, waste containing predominantly polyolefins can easily be broken down into low-molecular fragments in the presence of manganese, vanadium, copper, chromium, molybdenum or tungsten compounds at elevated temperatures.
  • the catalytically active metals can already be present in the plastics in the form of the additives, so that their addition is unnecessary.
  • the fission products boil in the area of crude gasoline (naphtha) and middle distillates and also have the viscosity of these petroleum fractions. They can therefore be pumped using conventional devices.
  • Hydrocarbons generated during the splitting partly leave the reactor as vapors in a mixture with hydrogen chloride and small amounts of other fission gases such as carbon monoxide, hydrogen, nitrogen and ammonia. They are obtained from the gaseous mixture by partial condensation as an ash-free condensate. It is a 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 contains all of the ash, is discharged in liquid form and converted into synthesis gas either alone or in a mixture with other raw materials, eg naphtha, with steam and oxygen.
  • This reaction can also be carried out by known methods. Processes that allow problem-free separation of the ashes and their extraction without external admixtures are particularly suitable.
  • the solution to this problem requires the highest possible carbon conversion in the reactor in order to avoid the discharge of soot together with the ash.
  • special cooling devices must be provided for the raw gas that carries liquid ash. Direct cooling with water in a quench cooler or a system consisting of a radiation cooler and a convection cooler has proven its worth. The cooling stage is followed by water washes, in which the last ash residues are removed.
  • the ashes can be stored in landfills or processed into metals.
  • the gasification itself takes place at temperatures between 1100 and 1500 ° C and a pressure of 1 to 10 MPa.
  • the raw gas leaving the gasification reactor at a temperature of 1300 to 1500 ° C. contains, in addition to soot, metals and / or metal compounds in the stated amount in liquid form. It is first pre-cooled in a radiation cooler to 500 to 1000 ° C, a 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, the remaining portion of fine metal particles and soot particles containing raw gas is passed into a convection cooler.
  • the carbon monoxide / hydrogen mixture obtained by gasification of 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 / H2 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 elimination of hydrogen chloride from chlorine-containing plastics, the hydrogen chloride is washed out with water from the reaction product and in a known manner, e.g. to 30% crude acid, worked up. In special cases, the hydrogen chloride can also be neutralized in an alkaline wash.
  • the splitting is followed by gasification, i.e. the partial oxidation of the depolymerized waste with oxygen in the presence of water vapor.
  • hydrogen can also be obtained from the raw gas.
  • it is converted, the resulting CO2 / H2 mixture is fed into a chemical wash and separated into CO2 and H2 in a pressure swing absorption stage.
  • Returned 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.
  • the liquid depolymerizate has the following composition.
  • N 0.4% by weight
  • 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 of depolymerized material 325 Nm3 of oxygen and 110 kg of steam are required.
  • the raw gas contains 43.8 vol .-% CO, 48.6 vol .-% H2 and 6.6 vol .-% CO2; the CO / H2 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 Procédé de préparation de gaz de synthèse Expired - Lifetime EP0639631B1 (fr)

Applications Claiming Priority (2)

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

Publications (2)

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

Family

ID=6495729

Family Applications (1)

Application Number Title Priority Date Filing Date
EP94112796A Expired - Lifetime EP0639631B1 (fr) 1993-08-21 1994-08-17 Procédé de préparation de gaz de synthèse

Country Status (10)

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

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
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
WO2023115083A1 (fr) * 2021-12-20 2023-06-29 Walter Kanzler Appareil de réacteur

Families Citing this family (19)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CA2260953A1 (fr) * 1996-07-17 1998-01-22 John Saunders Stevenson Oxydation partielle de dechets de matieres plastiques
WO2000059825A1 (fr) * 1999-04-02 2000-10-12 Ebara Corporation Procede et appareil de production d'hydrogene par gazeification de matiere combustible
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 (fr) * 2009-04-06 2013-08-28 Rentech Inc Système et procédé de conditionnement de gaz de synthèse dérivé de biomasse
EP2834323A4 (fr) * 2013-06-04 2015-10-07 Enviro Power Pte Ltd Système et procédé pour convertir une matière plastique/caoutchouc en carburant hydrocarboné par un procédé thermo-catalytique
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
US12157251B2 (en) 2020-02-10 2024-12-03 Eastman Chemical Company Waste plastic density separation
WO2021211521A1 (fr) * 2020-04-13 2021-10-21 Eastman Chemical Company Gazéification par oxydation partielle de déchets plastiques humides
BR112022020570A2 (pt) * 2020-04-13 2022-11-29 Eastman Chem Co Método para reciclar um resíduo plástico, e, uso de finos secos contendo tereftalato de polietileno
CA3174818A1 (fr) * 2020-04-13 2021-10-21 Bruce Roger Debruin Recyclage chimique de matieres de purge
CA3174721A1 (fr) * 2020-04-13 2021-10-21 Bruce Roger Debruin Recyclage chimique de melanges de plastiques contenant du metal
KR20240138616A (ko) 2023-03-09 2024-09-20 에스케이이노베이션 주식회사 합성가스 제조방법, 제조장치 및 이를 이용한 액상 탄화수소 제조방법

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DE2205001B1 (de) * 1972-02-03 1973-07-26 Ruhrchemie Ag, 4200 Oberhausen-Holten Verfahren zur thermischen aufbereitung von abfaellen aus kunststoff und kautschuk
FR2357630A1 (fr) * 1976-07-05 1978-02-03 Erap Procede perfectionne de craquage catalytique
US4108730A (en) * 1977-03-14 1978-08-22 Mobil Oil Corporation Method for treatment of rubber and plastic wastes

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DE2840987A1 (de) * 1978-09-21 1980-04-03 Linde Ag Verfahren zum spalten von kohlenwasserstoffen
JPS60219292A (ja) * 1984-04-13 1985-11-01 Mitsubishi Heavy Ind Ltd 石油化学製品の選択的製造法
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DE4017089C3 (de) * 1990-05-26 1996-10-17 Menges Georg Verfahren und Vorrichtung zum Vegasen von Kunststoffen zur Erzeugung von Synthesegas
DE4029880A1 (de) * 1990-09-21 1992-03-26 Menges Georg Verfahren zum vergasen von kunststoffen zur erzeugung von brenngasen
US5061363A (en) * 1990-10-09 1991-10-29 The United States Of America As Represented By The United States Department Of Energy Method for co-processing waste rubber and carbonaceous material
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DE4311034A1 (de) * 1993-04-03 1994-10-06 Veba Oel Ag Verfahren zur Gewinnung von Chemierohstoffen und Kraftstoffkomponenten aus Alt- oder Abfallkunststoff

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Publication number Priority date Publication date Assignee Title
DE2205001B1 (de) * 1972-02-03 1973-07-26 Ruhrchemie Ag, 4200 Oberhausen-Holten Verfahren zur thermischen aufbereitung von abfaellen aus kunststoff und kautschuk
FR2169965A1 (fr) * 1972-02-03 1973-09-14 Ruhrchemie Ag
FR2357630A1 (fr) * 1976-07-05 1978-02-03 Erap Procede perfectionne de craquage catalytique
US4108730A (en) * 1977-03-14 1978-08-22 Mobil Oil Corporation Method for treatment of rubber and plastic wastes

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
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
WO2023115083A1 (fr) * 2021-12-20 2023-06-29 Walter Kanzler Appareil de réacteur

Also Published As

Publication number Publication date
BR9403282A (pt) 1995-04-11
EP0639631B1 (fr) 1999-11-24
DE4328188C2 (de) 1996-04-18
CA2130019A1 (fr) 1995-02-22
DE4328188A1 (de) 1995-02-23
JPH07197041A (ja) 1995-08-01
KR100308464B1 (ko) 2001-12-01
KR950005959A (ko) 1995-03-20
ATE186940T1 (de) 1999-12-15
CA2130019C (fr) 1999-10-19
US5457250A (en) 1995-10-10
DE59408948D1 (de) 1999-12-30
TW310333B (fr) 1997-07-11
JP2534461B2 (ja) 1996-09-18
ES2141788T3 (es) 2000-04-01

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