EP2057252A1 - Method for producing fuels from waste - Google Patents

Method for producing fuels from waste

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Publication number
EP2057252A1
EP2057252A1 EP07801883A EP07801883A EP2057252A1 EP 2057252 A1 EP2057252 A1 EP 2057252A1 EP 07801883 A EP07801883 A EP 07801883A EP 07801883 A EP07801883 A EP 07801883A EP 2057252 A1 EP2057252 A1 EP 2057252A1
Authority
EP
European Patent Office
Prior art keywords
synthesis gas
reaction
waste
temperature
zone
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.)
Ceased
Application number
EP07801883A
Other languages
German (de)
French (fr)
Inventor
Günter H. KISS
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.)
Thermoselect AG
Original Assignee
Thermoselect AG
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Thermoselect AG filed Critical Thermoselect AG
Publication of EP2057252A1 publication Critical patent/EP2057252A1/en
Ceased legal-status Critical Current

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Classifications

    • 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
    • C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
    • C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
    • 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
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/48—Apparatus; Plants
    • C10J3/50—Fuel charging devices
    • C10J3/506—Fuel charging devices for entrained flow gasifiers
    • 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
    • C10J3/72—Other features
    • C10J3/721—Multistage gasification, e.g. plural parallel or serial gasification stages
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
    • C10K3/02—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment
    • C10K3/04—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment reducing the carbon monoxide content, e.g. water-gas shift [WGS]
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L5/00—Solid fuels
    • C10L5/02—Solid fuels such as briquettes consisting mainly of carbonaceous materials of mineral or non-mineral origin
    • C10L5/34—Other details of the shaped fuels, e.g. briquettes
    • C10L5/36—Shape
    • C10L5/361—Briquettes
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L5/00—Solid fuels
    • C10L5/40—Solid fuels essentially based on materials of non-mineral origin
    • C10L5/44—Solid fuels essentially based on materials of non-mineral origin on vegetable substances
    • 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
    • C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
    • C10G2300/10—Feedstock materials
    • C10G2300/1003—Waste materials
    • 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
    • C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
    • C10G2300/40—Characteristics of the process deviating from typical ways of processing
    • C10G2300/4081—Recycling aspects
    • 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
    • C10J2200/00—Details of gasification apparatus
    • C10J2200/15—Details of feeding means
    • 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
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0903—Feed preparation
    • 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
    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/0916—Biomass
    • 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
    • C10J2300/00—Details of gasification processes
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656—Conversion of synthesis gas to chemicals
    • C10J2300/1659—Conversion of synthesis gas to chemicals to liquid hydrocarbons
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/10—Biofuels, e.g. bio-diesel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/141—Feedstock
    • Y02P20/145—Feedstock the feedstock being materials of biological origin

Definitions

  • the present invention relates to a process in which synthesis gas is first generated from waste and the synthesis gas is subsequently converted into hydrocarbons.
  • the hydrocarbons produced can be used as fuels.
  • the best known method for the alternative production of fuel is the Fischer-Tropsch synthesis.
  • the Fischer-Tropsch process is one of Franz Fischer and his colleague Hans Tropsch in Mülheim an der Ruhr before 1925 developed large-scale process for the conversion of synthesis gas (CO / H 2 ) into liquid hydrocarbons. On a large scale, the process was applied from 1934 by Ruhrchemie AG. There is a build-up reaction of CO / H 2 mixtures of iron or cobalt catalysts to paraffins, olefins and alcohols.
  • Substantially linear hydrocarbon molecules The product mix has different chain lengths. Of particular interest for fuel production is the chain length range of C 5 -C 20 .
  • the chain length can be adjusted by catalyst selection (cobalt, iron, with promoters) and synthesis conditions (especially temperature, synthesis gas composition, pressure).
  • the primary Fischer-Tropsch synthesis products are then chemically processed in terms of high fuel yields and qualities (eg hydrocracking, isomerization, ie processes of petroleum processing).
  • the product Due to the peculiarity of the chemical synthesis mechanism to mainly low-branched hydrocarbon molecules, the product is mainly suitable as a high-quality diesel fuel with high cetane number and extremely low levels of sulfur and aromatics.
  • product mixtures with respect to different chain lengths of the hydrocarbons can be tailored in the
  • the Carbo-V ® process is a three-stage gasification process with the sub-processes:
  • the biomass (water content 15 - 20%) is continuously carbonated in the first process stage by partial oxidation (carbonization) with air or oxygen at temperatures between 400 and 500 0 C, ie in tar-containing gas (volatile constituents) and solid carbon (Biokoks ) decomposed.
  • the tar-containing gas is nachoxi- diert in a combustion chamber above the ash melting point of the fuel with air and / or oxygen under stoichiometric to hot gasification agent.
  • the biofuel ground to the fuel dust is injected into the hot gasification agent.
  • combustible dust and gasification agent in the gasification reactor react endothermically to synthesis crude gas. This can then be tion as fuel gas for electricity, steam and heat generation or as synthesis gas with the aid of the Fischer-Tropsch process for the production of SunDiesel.
  • Disadvantages of this method are that the gasification takes place in several stages and the biocok must be ground up. In addition, this method is not suitable for the gasification of waste of all kinds.
  • Waste and subsequent synthesis of fuels allowed, where possible, the entire waste can be used.
  • a method for the disposal and use of waste of all kinds, in which the waste is subjected to zone-wise temperature and thermal separation or conversion and the resulting solid residues are transferred to a high-temperature melt, the waste is compressed in batches to form compact packages and Temperature treatment zones, with at least one low-temperature zone and at least one high-temperature zone, in which synthesis gas is generated from the waste, go through in the direction of rising temperature, the synthesis gas generated passes through a gas-permeable bed and located above the bed stabilization zone for the synthesis gas and then is derived from the stabilizing zone, wherein the synthesis gas is reacted in a subsequent reaction to hydrocarbon molecules.
  • the reaction product is fuel, more preferably diesel fuel.
  • a significant advantage of the method is that now waste of all kinds, i. treated, untreated, pollutant and special waste as well as biowaste, without prior elaborate separation in the inventive method can be used.
  • Such a method is known in the art as Thermoselect method and is for example in European patents EP 1 187 891 Bl, EP 1 252 264 Bl, EP 1 377 358 Bl, EP 0 790 291 Bl or EP 0 726 307 Bl closer described. The full disclosure of these European patents is hereby incorporated by reference.
  • the method provides that at least 70%, preferably 100% of the synthesis gas generated is used for the reaction to hydrocarbons.
  • the unused portion of synthesis gas is advantageously used to cover the energy consumption of the disposal process.
  • the gaseous, liquid and / or solid by-products resulting from the reaction of the synthesis gas with hydrocarbons are introduced into the high-temperature Returned to the synthesis gas production zone, so that the Fischer-Tropsch synthesis without additional waste, which would have to be disposed of subsequently, executable.
  • the by-products of the Fischer-Tropsch synthesis are used to meet the energy requirements of the disposal process.
  • the reaction is known in the art as the Fischer-Tropsch process.
  • the known in the art in the state of
  • the process is controlled such that the hydrocarbons have on average 5 to 20 carbon atoms and are as unbranched as possible.
  • the hydrocarbons have on average 5 to 20 carbon atoms and are as unbranched as possible.
  • the Fischer-Tropsch synthesis the synthesis of longer-chain hydrocarbons is generally possible;
  • longer-chain hydrocarbons eg paraffins, have too high a melting point to be used as a liquid fuel.
  • Hydrocarbons which have an average of 5 to 20 carbon atoms, however, are outstandingly suitable for use as a synthetic diesel fuel.
  • the synthesis gas obtained from the gasification process for the Fischer-Tropsch process has a relatively unfavorable volume ratio of carbon monoxide to hydrogen, it is also advantageous if, before the polymerization reaction, the volume ratio of carbon monoxide to hydrogen is shifted in favor of hydrogen in a shift reaction.
  • This shift reaction is also known to those skilled in the art; Reference is made to the optimized reaction conditions and catalysts used.
  • the volume ratio of carbon monoxide to hydrogen in the shift reaction is set to at least 1: 1.5, preferably at least 1: 2.
  • the process can be used for the synthesis of fuels, preferably for the synthesis of diesel fuels.
  • the process according to the invention is explained in more detail by means of a Thermoselect plant, which has two lines each with 15 t / h waste throughput, ie a total of 30 t / h waste throughput possible. This results in an average waste heat value of 12 MJ / kg Based on waste.
  • H 2 and 14% CO 2 by volume are obtained approximately 30,000 Nm 3 / h of synthesis gas of the composition of 38% by volume of CO, by volume of 38. 1
  • the fuel is produced according to the Fischer-Tropsch process.
  • a portion of the CO is converted to H 2 in a shift reaction.
  • the resulting CO 2 is separated.

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  • Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • General Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Environmental & Geological Engineering (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Geochemistry & Mineralogy (AREA)
  • Geology (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Processing Of Solid Wastes (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

The invention relates to a method for disposal and reclamation of waste materials of all types, wherein the waste materials are compressed in batches into compact packages and run through temperature treatment zones, to give synthesis gas and the synthesis gas is transformed in a further reaction to give hydrocarbon molecules.

Description

Verfahren zur Erzeugung von Kraftstoffen aus Abfall Process for the production of fuels from waste
Vorliegende Erfindung betrifft ein Verfahren, bei dem aus Abfall zunächst Synthesegas erzeugt und das Syn- thesegas anschließend zu Kohlenwasserstoffen umgesetzt wird. Die erzeugten Kohlenwasserstoffe können als Kraftstoffe verwendet werden.The present invention relates to a process in which synthesis gas is first generated from waste and the synthesis gas is subsequently converted into hydrocarbons. The hydrocarbons produced can be used as fuels.
Die Entwicklung des Ölpreises in den letzten Jahren ging immer weiter nach oben. Auch wenn der Ölpreis zwischendurch teilweise fällt, ist langfristig von einem hohen Ölpreis auszugehen, so dass alternative Verfahren zur Herstellung von Treibstoff zukünftig immer interessanter werden.The development of the oil price in recent years has continued to rise. Even if the price of oil falls partially in the long run, a high oil price is expected in the long term, so that alternative processes for the production of fuel will become increasingly interesting in the future.
Bekanntestes Verfahren zur alternativen Herstellung von Treibstoff ist die Fischer-Tropsch-Synthese . Das Fischer-Tropsch-Verfahren ist ein von Franz Fischer und seinem Mitarbeiter Hans Tropsch in Mülheim an der Ruhr vor 1925 entwickeltes großtechnisches Verfahren zur Umwandlung von Synthesegas (CO/H2) in flüssige Kohlenwasserstoffe. Großtechnisch wurde das Verfahren ab 1934 von der Ruhrchemie AG angewandt. Es ist eine Aufbaureaktion von CO/H2-Gemischen an Eisen- oder Cobalt-Katalysatoren zu Paraffinen, Alkenen und Alkoholen.The best known method for the alternative production of fuel is the Fischer-Tropsch synthesis. The Fischer-Tropsch process is one of Franz Fischer and his colleague Hans Tropsch in Mülheim an der Ruhr before 1925 developed large-scale process for the conversion of synthesis gas (CO / H 2 ) into liquid hydrocarbons. On a large scale, the process was applied from 1934 by Ruhrchemie AG. There is a build-up reaction of CO / H 2 mixtures of iron or cobalt catalysts to paraffins, olefins and alcohols.
Der chemische Mechanismus der Fischer-Tropsch Synthesereaktion (Polymerisation) führt hauptsächlich zu langkettigen, gering verzweigten (d.h. imThe chemical mechanism of the Fischer-Tropsch synthesis reaction (polymerization) results mainly in long-chain, low-branched (i.e.
Wesentlichen linearen) Kohlenwasserstoff-Molekülen. In der Produktmischung finden sich unterschiedliche Kettenlängen. Für die Treibstoffherstellung besonders interessant ist der Kettenlängenbereich von C5-C20. Die Kettenlänge kann durch Katalysatorwahl (Kobalt, Eisen, mit Promotoren) und Synthesebedingungen (vor allem Temperatur, Synthesegas-Zusammensetzung, Druck) eingestellt werden. Die primären Fischer-Tropsch- Syntheseprodukte werden dann im Sinne hoher Kraft- stoff-Ausbeuten und -Qualitäten chemisch aufgearbeitet (z.B. Hydrocracken, Isomerisieren, d.h. Verfahren der Erdölverarbeitung) .Substantially linear) hydrocarbon molecules. The product mix has different chain lengths. Of particular interest for fuel production is the chain length range of C 5 -C 20 . The chain length can be adjusted by catalyst selection (cobalt, iron, with promoters) and synthesis conditions (especially temperature, synthesis gas composition, pressure). The primary Fischer-Tropsch synthesis products are then chemically processed in terms of high fuel yields and qualities (eg hydrocracking, isomerization, ie processes of petroleum processing).
Aufgrund der Besonderheit des chemischen Synthese- mechanismus zu hauptsächlich gering verzweigten Kohlenwasserstoff-Molekülen eignet sich das Produkt vor allem als hochwertiger Dieselkraftstoff mit hoher Cetanzahl und extrem niedrigen Gehalten an Schwefel und Aromaten. Produktmischungen hinsichtlich unterschiedlicher Kettenlänge der Kohlenwasserstoffe können darüber hinaus maßgeschneidert werden imDue to the peculiarity of the chemical synthesis mechanism to mainly low-branched hydrocarbon molecules, the product is mainly suitable as a high-quality diesel fuel with high cetane number and extremely low levels of sulfur and aromatics. In addition, product mixtures with respect to different chain lengths of the hydrocarbons can be tailored in the
Hinblick auf Dampfdruck, Siedeverläufe u.a. unter Anwendung der hochentwickelten Erdöl-Raffinerieverfahren. Diese synthetisch hergestellten Diesel- kraftstoffe haben den Vorteil besonders Schadstoffarm und damit umweltfreundlich zu sein.With regard to vapor pressure, boiling characteristics, etc., using sophisticated petroleum refining processes. These synthetically manufactured diesel fuels have the advantage of being low in pollutants and therefore environmentally friendly.
Momentan ist Südafrika das einzige Land, das einen Großteil seines Treibstoffbedarfs durch die Fischer- Tropsch-Reaktion deckt. Dort wird das Synthesegas für die Synthese aus Kohle hergestellt.South Africa is currently the only country that covers most of its fuel needs through the Fischer-Tropsch reaction. There, the synthesis gas for the synthesis of coal is produced.
In Deutschland hat das Unternehmen Choren ein Verfahren entwickelt, um aus Biomasse mit dem Carbo-V-Ver- fahren erst Synthesegas und dann mit Hilfe des Fischer-Tropsch-Verfahrens Treibstoff (sog.In Germany, the company Choren has developed a process to convert biomass with the Carbo-V process first into syngas and then with the help of the Fischer-Tropsch process fuel (so-called "gas").
SunDiesel) herzustellen. Das Carbo-V®-Verfahren ist ein dreistufiges Vergasungsverfahren mit den Teilprozessen :SunDiesel). The Carbo-V ® process is a three-stage gasification process with the sub-processes:
• Niedertemperaturvergasung, • Hochtemperaturvergasung und• low temperature gasification, • high temperature gasification and
• endotherme Flugstromvergasung.• endothermic entrained flow gasification.
Die Biomasse (Wassergehalt 15 - 20 %) wird in der ersten Prozess-Stufe kontinuierlich durch partielle Oxidation (Verschwelung) mit Luft oder Sauerstoff bei Temperaturen zwischen 400 und 500 0C karbonisiert, d.h. in teerhaltiges Gas (flüchtige Bestandteile) und festen Kohlenstoff (Biokoks) zerlegt.The biomass (water content 15 - 20%) is continuously carbonated in the first process stage by partial oxidation (carbonization) with air or oxygen at temperatures between 400 and 500 0 C, ie in tar-containing gas (volatile constituents) and solid carbon (Biokoks ) decomposed.
In der zweiten Prozess-Stufe wird das teerhaltige Gas in einer Brennkammer oberhalb des Ascheschmelzpunktes der Brennstoffe mit Luft und/oder Sauerstoff unter- stöchiometrisch zu heißem Vergasungsmittel nachoxi- diert .In the second process stage, the tar-containing gas is nachoxi- diert in a combustion chamber above the ash melting point of the fuel with air and / or oxygen under stoichiometric to hot gasification agent.
In der dritten Prozess-Stufe wird der zu Brennstaub gemahlene Biokoks in das heiße Vergasungsmittel eingeblasen. Dabei reagieren Brennstaub und Vergasungsmittel im Vergasungsreaktor endotherm zu Synthese-Rohgas. Dieses kann dann nach entsprechender Kon- ditionierung als Brenngas zur Strom-, Dampf- und Wärmeerzeugung oder als Synthesegas mit Hilfe des Fischer-Tropsch-Verfahrens für die SunDiesel-Herstel- lung genutzt werden. Nachteile dieses Verfahrens sind, dass die Vergasung in mehreren Stufen abläuft und der Biokoks aufgemahlen werden muss . Außerdem eignet sich dieses Verfahren nicht zur Vergasung von Abfällen aller Art.In the third stage of the process, the biofuel ground to the fuel dust is injected into the hot gasification agent. In this process, combustible dust and gasification agent in the gasification reactor react endothermically to synthesis crude gas. This can then be tion as fuel gas for electricity, steam and heat generation or as synthesis gas with the aid of the Fischer-Tropsch process for the production of SunDiesel. Disadvantages of this method are that the gasification takes place in several stages and the biocok must be ground up. In addition, this method is not suitable for the gasification of waste of all kinds.
Somit ist es Aufgabe vorliegender Erfindung, ein Verfahren bereitzustellen, das eine Vergasung vonThus, it is an object of the present invention to provide a method that gasification of
Abfall sowie anschließende Synthese von Kraftstoffen erlaubt, wobei möglichst der gesamte Abfall genutzt werden kann.Waste and subsequent synthesis of fuels allowed, where possible, the entire waste can be used.
Diese Aufgabe wird durch das Verfahren mit den Merkmalen des Anspruchs 1 gelöst. Ein möglicher Verwendungszweck des Verfahrens wird in Patentanspruch 10 gegeben. Die abhängigen Ansprüche bilden dabei vorteilhafte Weiterbildungen.This object is achieved by the method having the features of claim 1. A possible use of the method is given in claim 10. The dependent claims form advantageous developments.
Erfindungsgemäß wird ein Verfahren zur Entsorgung und Nutzung von Abfallgütern aller Art bereitgestellt, bei dem die Abfallgüter einer zonenweisen Temperaturbeaufschlagung und thermischen Trennung bzw. Stoffum- Wandlung unterzogen und die anfallenden festen Rückstände in eine Hochtemperaturschmelze überführt werden, wobei die Abfallgüter chargenweise zu Kompaktpaketen komprimiert werden und Temperaturbehandlungszonen, mit mindestens einer Niedertemperaturzone und mindestens einer Hochtemperaturzone, in der aus dem Entsorgungsgut Synthesegas erzeugt wird, in Richtung steigender Temperatur durchlaufen, das erzeugte Synthesegas eine gasdurchlässige Schüttung sowie eine oberhalb der Schüttung befindliche Stabilisierungszo- ne für die Synthesegase durchläuft und anschließend aus der Stabilisierungszone abgeleitet wird, wobei das Synthesegas in einer anschließenden Reaktion zu Kohlenwasserstoff-Molekülen umgesetzt wird. Bevorzugt handelt es sich bei dem Reaktionsprodukt um Kraftstoff, besonders bevorzugt um Dieselkraftstoff.According to the invention, a method is provided for the disposal and use of waste of all kinds, in which the waste is subjected to zone-wise temperature and thermal separation or conversion and the resulting solid residues are transferred to a high-temperature melt, the waste is compressed in batches to form compact packages and Temperature treatment zones, with at least one low-temperature zone and at least one high-temperature zone, in which synthesis gas is generated from the waste, go through in the direction of rising temperature, the synthesis gas generated passes through a gas-permeable bed and located above the bed stabilization zone for the synthesis gas and then is derived from the stabilizing zone, wherein the synthesis gas is reacted in a subsequent reaction to hydrocarbon molecules. Preferably, the reaction product is fuel, more preferably diesel fuel.
Ein wesentlicher Vorteil des Verfahrens ist es, dass nunmehr Abfallgüter aller Art, d.h. behandelter, unbehandelter, Schadstoff- und sondermüllhaltiger sowie Bioabfall, ohne vorherige aufwändige Trennung beim erfindungsgemäßen Verfahren eingesetzt werden kann. Ein derartiges Verfahren ist im Stand der Technik als Thermoselect-Verfahren bekannt und wird beispielsweise in den europäischen Patenten EP 1 187 891 Bl, EP 1 252 264 Bl, EP 1 377 358 Bl, EP 0 790 291 Bl oder EP 0 726 307 Bl näher beschrieben. Der komplette Offenbarungsgehalt dieser europäischen Patente wird hiermit eingeschlossen.A significant advantage of the method is that now waste of all kinds, i. treated, untreated, pollutant and special waste as well as biowaste, without prior elaborate separation in the inventive method can be used. Such a method is known in the art as Thermoselect method and is for example in European patents EP 1 187 891 Bl, EP 1 252 264 Bl, EP 1 377 358 Bl, EP 0 790 291 Bl or EP 0 726 307 Bl closer described. The full disclosure of these European patents is hereby incorporated by reference.
In einer vorteilhaften Weiterbildung sieht das Verfahren vor, dass mindestens 70 %, bevorzugt 100 % des erzeugten Synthesegases zur Reaktion zu Kohlenwasserstoffen genutzt wird. Dabei wird vorteilhafterweise der nicht genutzte Anteil an Synthesegas zur Deckung des energetischen Eigenbedarfs des Entsorgungsverfahrens verwendet. Dies bringt den Vorteil mit sich, dass eine neutrale Energiebilanz des Verfahrens gewährleistet ist. Weiterhin ist es ein wesentlicher Vorteil des Verfahrens, dass ein quasi emissionsfreier Ablauf gewährleistet ist.In an advantageous embodiment, the method provides that at least 70%, preferably 100% of the synthesis gas generated is used for the reaction to hydrocarbons. In this case, the unused portion of synthesis gas is advantageously used to cover the energy consumption of the disposal process. This has the advantage that a neutral energy balance of the process is guaranteed. Furthermore, it is a significant advantage of the method that a quasi-emission-free process is guaranteed.
In einer weiteren bevorzugten Ausführungsform werden die bei der Reaktion des Synthesegases zu Kohlenwasserstoffen anfallenden gasförmigen, flüssigen und/oder festen Nebenprodukte in die Hochtemperatur- zone der Synthesegaserzeugung zurückgeführt, so dass auch die Fischer-Tropsch-Synthese ohne weitere Abfälle, die nachträglich entsorgt werden müssten, ausführbar ist.In a further preferred embodiment, the gaseous, liquid and / or solid by-products resulting from the reaction of the synthesis gas with hydrocarbons are introduced into the high-temperature Returned to the synthesis gas production zone, so that the Fischer-Tropsch synthesis without additional waste, which would have to be disposed of subsequently, executable.
In einer weiteren bevorzugten Ausführungsform werden die Nebenprodukte der Fischer-Tropsch-Synthese zur Deckung des energetischen Eigenbedarfs des Entsorgungsverfahrens verwendet .In a further preferred embodiment, the by-products of the Fischer-Tropsch synthesis are used to meet the energy requirements of the disposal process.
Zur Erzielung von guten Ausbeuten ist es günstig, wenn die Reaktion in einem Temperaturbereich von 200 0C bis 350 0C und Drücken von 10 - 30 bar gemäß der allgemeinen ReaktionsgleichungTo obtain good yields, it is advantageous if the reaction in a temperature range of 200 0 C to 350 0 C and pressures of 10 - 30 bar according to the general reaction equation
πCO + ( 2n+l ) H2 → CnH2n+2 + ^H2OπCO + (2n + 1) H 2 → C n H 2n + 2 + ^ H 2 O
durchgeführt wird. Die Reaktion ist im Stand der Technik als Fischer-Tropsch-Verfahren bekannt. Dazu wird auf die dem Fachmann bekannten, im Stand deris carried out. The reaction is known in the art as the Fischer-Tropsch process. For this purpose, the known in the art, in the state of
Technik erwähnten optimierten Verfahrensbedingungen verwiesen, wie z.B. Druck, Temperaturen und Katalysatorensysteme .Referred to optimized process conditions, such as Pressure, temperatures and catalyst systems.
Weiterhin ist es vorteilhaft, wenn das Verfahren so gesteuert wird, dass die Kohlenwasserstoffe im Mittel 5 bis 20 Kohlenstoffatome aufweisen und möglichst unverzweigt sind. Mit der Fischer-Tropsch-Synthese ist generell auch die Synthese von längerkettigen Kohlen- Wasserstoffen möglich; längerkettige Kohlenwasserstoffe, z.B. Paraffine, weisen jedoch einen zu hohen Schmelzpunkt auf, um als flüssiger Kraftstoff eingesetzt werden zu können. Kohlenwasserstoffe, die im Mittel 5 bis 20 Kohlenstoffatome aufweisen, eigenen sich hingegen hervorragend zum Einsatz als synthetischer Dieselkraftstoff. Da das aus dem Vergasungsverfahren erhaltene Synthesegas für das Fischer-Tropsch-Verfahren ein relativ ungünstiges Volumenverhältnis von Kohlenmonoxid zu Wasserstoff aufweist, ist es weiterhin vorteilig, wenn vor der Polymerisationsreaktion das Volumenverhältnis von Kohlenmonoxid zu Wasserstoff in einer Shift-Reaktion zugunsten von Wasserstoff verschoben wird. Diese Shift-Reaktion ist dem Fachmann aus dem Stand der Technik ebenfalls bekannt; es wird auf die optimierten Reaktionsbedingungen und verwendeten Katalysatoren verwiesen.Furthermore, it is advantageous if the process is controlled such that the hydrocarbons have on average 5 to 20 carbon atoms and are as unbranched as possible. With the Fischer-Tropsch synthesis, the synthesis of longer-chain hydrocarbons is generally possible; However, longer-chain hydrocarbons, eg paraffins, have too high a melting point to be used as a liquid fuel. Hydrocarbons, which have an average of 5 to 20 carbon atoms, however, are outstandingly suitable for use as a synthetic diesel fuel. Since the synthesis gas obtained from the gasification process for the Fischer-Tropsch process has a relatively unfavorable volume ratio of carbon monoxide to hydrogen, it is also advantageous if, before the polymerization reaction, the volume ratio of carbon monoxide to hydrogen is shifted in favor of hydrogen in a shift reaction. This shift reaction is also known to those skilled in the art; Reference is made to the optimized reaction conditions and catalysts used.
In einer weiteren zu bevorzugenden Ausführungsform wird dabei das Volumenverhältnis von Kohlenmonoxid zu Wasserstoff in der Shift-Reaktion auf mindestens 1 zu 1,5, bevorzugt mindestens 1 zu 2 eingestellt.In a further preferred embodiment, the volume ratio of carbon monoxide to hydrogen in the shift reaction is set to at least 1: 1.5, preferably at least 1: 2.
Weiterhin wird mit vorliegender Erfindung eine Ver- wendung des voranstehend beschriebenen Verfahrens angegeben. Erfindungsgemäß kann das Verfahren zur Synthese von Treibstoffen, bevorzugt zur Synthese von Dieselkraftstoffen, verwendet werden.Furthermore, a use of the method described above is specified with the present invention. According to the invention, the process can be used for the synthesis of fuels, preferably for the synthesis of diesel fuels.
Im nachfolgenden wird erfindungsgemäßes Verfahren anhand eines Beispiels näher erläutert, ohne die Erfindung auf die dort verwendeten Verfahrensparameter zu beschränken.In the following, method according to the invention will be explained in more detail by means of an example, without limiting the invention to the method parameters used there.
Beispiel zur VerfahrensführungExample of process control
Das erfindungsgemäße Verfahren wird anhand einer Thermoselect-Anlage näher erläutert, die zwei Linien mit je 15 t/h Abfalldurchsatz aufweist, d.h. insge- samt 30 t/h Abfalldurchsatz ermöglicht. Dabei wird ein durchschnittlicher Abfallheizwert von 12 MJ/kg Abfall zugrunde gelegt. Bei einer kontinuierlichen Betreibung der Anlage können dabei ca. 30.000 Nm3/h Synthesegas der Zusammensetzung 38 VoI-% CO, 38 VoI-1 H2 und 14 Vol-% CO2 erhalten werden. Die Treibstoffherstellung erfolgt gemäß des Fischer-Tropsch- Verfahrens . Um ein für die Fischer-Tropsch-Reaktion günstiges CO/H2-Verhältnis einzustellen, wird in einer Shift-Reaktion ein Teil des CO zu H2 konvertiert. Das hierbei entstehende CO2 wird abgetrennt.The process according to the invention is explained in more detail by means of a Thermoselect plant, which has two lines each with 15 t / h waste throughput, ie a total of 30 t / h waste throughput possible. This results in an average waste heat value of 12 MJ / kg Based on waste. In a continuous management of the system can thereby H 2 and 14% CO 2 by volume are obtained approximately 30,000 Nm 3 / h of synthesis gas of the composition of 38% by volume of CO, by volume of 38. 1 The fuel is produced according to the Fischer-Tropsch process. In order to set a favorable for the Fischer-Tropsch reaction CO / H 2 ratio, a portion of the CO is converted to H 2 in a shift reaction. The resulting CO 2 is separated.
CO + H2O -> H2 + CO2 CO + H 2 O -> H 2 + CO 2
Von den 38 % CO im Synthesegases werden 13 % CO in der Shift-Reaktion umgesetzt, d.h. nach der Shift-Reaktion erhält man ein Synthesegas mit 25 % CO und 51 % H2, das dann in die Fischer-Tropsch-Synthese einge- setzt wird. Das so mit Wasserstoff angereicherte, auf ein für die Fischer-Tropsch-Reaktion günstiges Verhältnis von CO zu H2 gebrachte Synthesegas wird nun zu Dieselkraftstoff polymerisiertOf the 38% CO in the synthesis gas, 13% CO are converted in the shift reaction, ie after the shift reaction, a synthesis gas containing 25% CO and 51% H 2 is obtained , which is then used in the Fischer-Tropsch synthesis becomes. The thus enriched with hydrogen, to a favorable for the Fischer-Tropsch reaction ratio of CO to H 2 brought synthesis gas is now polymerized to diesel fuel
25 % CO + 51 % H2 => "Diesel"25% CO + 51% H 2 =>"Diesel"
Als Ausbeute über alle Stufen der Treibstoffherstellung wurden 60 % des eingesetzten Synthesegases erzielt. Dies liegt sehr nahe am Literaturwert, der für ein optimiertes Verfahren unter Laborbedingungen 75 % angibt. Für die Berechnung der Massenbilanz wurden die spezifischen Raumgewichte von CO und Wasserstoff zugrunde gelegt. Die Gleichung ist im Folgenden angegebenAs a yield over all stages of the fuel production 60% of the synthesis gas used were achieved. This is very close to the literature value, which indicates 75% for an optimized process under laboratory conditions. For the calculation of the mass balance, the specific volume weights of CO and hydrogen were used. The equation is given below
21 . 000 m3/h' ( 0 , 25 1 , 258 kg/m3 + 0 , 51 ' 0 , 089 kg/m3 ) =7557 kg/h21. 000 m 3 / h '(0, 25 1, 258 kg / m 3 + 0, 51' 0, 089 kg / m 3 ) = 7557 kg / h
Bei einer durchschnittlichen Dichte von 0,83 kg/1 des synthetischen Diesels ergibt sich somit eine Menge von 7.800 l/h Diesel. Mit einer 2-Linien-Thermo- select-Anlage können also 7.800 Liter Diesel pro Stunde produziert werden. With an average density of 0.83 kg / 1 of the synthetic diesel, this results in a lot of 7,800 l / h diesel. With a 2-line thermo-select system, 7,800 liters of diesel per hour can be produced.

Claims

Patentansprüche claims
1. Verfahren zur Entsorgung und Nutzbarmachung von Abfallgütern aller Art, bei dem die Abfallgüter einer zonenweisen Temperaturbeaufschlagung und thermischen Trennung bzw. StoffumWandlung unterzogen und die anfallenden festen Rückstände in eine Hochtemperaturschmelze überführt werden, wobei die Abfallgüter chargenweise zu Kompaktpaketen komprimiert werden und Temperaturbehand- lungszonen, mit mindestens einer Niedertemperaturzone und mindestens einer Hochtemperaturzone, in der aus dem Entsorgungsgut Synthesegas erzeugt wird, in Richtung steigender Temperatur durchlaufen, das erzeugte Synthesegas eine gas- durchlässige Schüttung sowie eine oberhalb der1. A method for disposal and utilization of waste of all kinds, in which the waste is subjected to a zone-wise temperature application and thermal separation or material conversion and the resulting solid residues are transferred to a high-temperature melt, the waste is compressed in batches to form compact packages and temperature treatment zones, with at least one low-temperature zone and at least one high-temperature zone, in which synthesis gas is produced from the waste material, in the direction of increasing temperature, the synthesis gas produced a gas-permeable bed and one above the
Schüttung befindliche Stabilisierungszone für die Synthesegase durchläuft und anschließend aus der Stabilisierungszone abgeleitet wird,Passes through the stabilization zone for the synthesis gas and is then discharged from the stabilization zone,
d a d u r c h g e k e n n z e i c h n e t,characterized,
dass das Synthesegas in einer anschließenden Reaktion zu Kohlenwasserstoff-Molekülen umgesetzt wird.that the synthesis gas is reacted in a subsequent reaction to hydrocarbon molecules.
2. Verfahren nach Anspruch 1, dadurch gekennzeichnet, dass mindestens 70 %, bevorzugt 80 %, ganz besonders bevorzugt 100 % des erzeugten Synthesegases zur Reaktion zu Kohlenwasserstoffen genutzt wird. 2. The method according to claim 1, characterized in that at least 70%, preferably 80%, very particularly preferably 100% of the synthesis gas generated is used for the reaction to hydrocarbons.
3. Verfahren nach vorhergehendem Anspruch, dadurch gekennzeichnet, dass der nicht zur Reaktion genutzte Anteil an Synthesegas zur Deckung des energetischen Eigenbedarfs des Entsorgungsver- fahrens verwendet wird.3. Method according to the preceding claim, characterized in that the proportion of synthesis gas not used for the reaction is used to cover the energy consumption of the disposal process.
4. Verfahren nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die bei der Reaktion anfallenden gasförmigen, flüssigen und/oder festen Nebenprodukte in die mindestens eine Hochtemperaturzone der Synthesegaserzeugung zurückgeführt werden.4. The method according to any one of the preceding claims, characterized in that the obtained in the reaction gaseous, liquid and / or solid by-products are recycled to the at least one high-temperature zone of synthesis gas production.
5. Verfahren nach Anspruch 4, dadurch gekennzeichnet, dass die rückgeführten Nebenprodukte zur Deckung des energetischen Eigenbedarfs des Ent- sorgungsverfahrens eingesetzt werden.5. The method according to claim 4, characterized in that the recycled by-products are used to cover the energy consumption of the waste disposal process.
6. Verfahren nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die Reaktion in einem Temperaturbereich von 200 0C bis 350 0C gemäß der allgemeinen Reaktionsgleichung nCO + ( 2π+l ) H2 → CnH2n+2 + πH2O durchgeführt wird .6. The method according to any one of the preceding claims, characterized in that the reaction in a temperature range from 200 0 C to 350 0 C according to the general reaction equation nCO + (2π + l) H 2 → C n H 2n + 2 + πH 2 O carried out becomes .
7. Verfahren nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass die Kohlenwasserstoffe im Mittel 5 bis 20 Kohlenstoffatome aufweisen.7. The method according to any one of the preceding claims, characterized in that the hydrocarbons have on average 5 to 20 carbon atoms.
8. Verfahren nach einem der vorhergehenden Ansprüche, dadurch gekennzeichnet, dass das Volumenverhältnis von Kohlenmonoxid zu Wasserstoff des Synthesegases vor der Reaktion in einer Shift- Reaktion zu Gunsten von Wasserstoff verschoben wird. 8. The method according to any one of the preceding claims, characterized in that the volume ratio of carbon monoxide to hydrogen of the synthesis gas is shifted before the reaction in a shift reaction in favor of hydrogen.
9. Verfahren nach vorhergehendem Anspruch, dadurch gekennzeichnet, dass das Volumenverhältnis von Kohlenmonoxid zu Wasserstoff nach der Shift- Reaktion mindestens 1 : 1,5, bevorzugt mindes- tens 1 : 2 beträgt .9. The method according to the preceding claim, characterized in that the volume ratio of carbon monoxide to hydrogen after the shift reaction is at least 1: 1.5, preferably at least 1: 2.
10. Verwendung des Verfahrens nach einem der vorhergehenden Ansprüche zur Synthese von Treibstoff.10. Use of the method according to any one of the preceding claims for the synthesis of fuel.
11. Verwendung nach vorhergehendem Anspruch, dadurch gekennzeichnet, dass der Treibstoff Dieselkraft- stoff ist. 11. Use according to the preceding claim, characterized in that the fuel is diesel fuel.
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Effective date: 20131115