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WO2008013794A2 - Conversion de matières carbonées en gaz naturel de synthèse par pyrolyse, reformage et méthanation - Google Patents

Conversion de matières carbonées en gaz naturel de synthèse par pyrolyse, reformage et méthanation Download PDF

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Publication number
WO2008013794A2
WO2008013794A2 PCT/US2007/016616 US2007016616W WO2008013794A2 WO 2008013794 A2 WO2008013794 A2 WO 2008013794A2 US 2007016616 W US2007016616 W US 2007016616W WO 2008013794 A2 WO2008013794 A2 WO 2008013794A2
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zone
product stream
methanation
pyrolysis
synthetic
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PCT/US2007/016616
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English (en)
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WO2008013794A3 (fr
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Stanley R. Pearson
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Clean Energy, L.L.C.
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Publication of WO2008013794A2 publication Critical patent/WO2008013794A2/fr
Publication of WO2008013794A3 publication Critical patent/WO2008013794A3/fr

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    • 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
    • C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/08—Production of synthetic natural gas
    • C—CHEMISTRY; METALLURGY
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    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/466—Entrained flow processes
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    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/58—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels combined with pre-distillation of the fuel
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    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/58—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels combined with pre-distillation of the fuel
    • C10J3/60—Processes
    • C10J3/64—Processes with decomposition of the distillation products
    • C10J3/66—Processes with decomposition of the distillation products by introducing them into the gasification zone
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    • C10K1/10—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors with aqueous liquids
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    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/08—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors
    • C10K1/10—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors with aqueous liquids
    • C10K1/12—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors with aqueous liquids alkaline-reacting including the revival of the used wash liquors
    • C10K1/14—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors with aqueous liquids alkaline-reacting including the revival of the used wash liquors organic
    • C10K1/143—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors with aqueous liquids alkaline-reacting including the revival of the used wash liquors organic containing amino groups
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    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/08—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors
    • C10K1/16—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors with non-aqueous liquids
    • C10K1/165—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors with non-aqueous liquids at temperatures below zero degrees Celsius
    • 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
    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/08—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors
    • C10K1/16—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors with non-aqueous liquids
    • C10K1/18—Purifying combustible gases containing carbon monoxide by washing with liquids; Reviving the used wash liquors with non-aqueous liquids hydrocarbon oils
    • C—CHEMISTRY; METALLURGY
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    • C10K1/00—Purifying combustible gases containing carbon monoxide
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    • C—CHEMISTRY; METALLURGY
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    • 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
    • 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
    • C10K3/026—Increasing the carbon monoxide content, e.g. reverse water-gas shift [RWGS]
    • 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
    • C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/10—Working-up natural gas or synthetic natural gas
    • C10L3/101—Removal of contaminants
    • C10L3/102—Removal of contaminants of acid contaminants
    • C—CHEMISTRY; METALLURGY
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    • 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
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    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
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    • C10J2300/093—Coal
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
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    • 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
    • C10J2300/1662—Conversion of synthesis gas to chemicals to methane
    • 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
    • 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 the production of synthetic natural gas from a carbonaceous material, preferably a biomass material, such as wood.
  • the carbonaceous material is first pyrolyzed, then subjected to steam reforming to produce a syngas, which is then passed to several clean-up steps then to a methanation zone to produce synthetic natural gas.
  • Synthetic natural gas A large portion of synthetic natural gas is often referred to as "green gas” because it is a renewable gas typically obtained from biomass and having natural gas specifications. Thus, it can be transported through the existing natural gas infrastructure, substituting for natural gas in all existing applications. Also, the use of biomass as the feedstock will not generally result in a net CO 2 emission as long as the source material can be replanted to replace those used as fuel. It may even be possible to reduce atmospheric CO 2 by sequestering the CO 2 that is released during the conversion of biomass (negative CO 2 emission).
  • the carbonaceous material is selected from the group consisting of wood and dried distillers grains.
  • Figure 1 hereof is a generalized flow scheme of a preferred embodiment of the present invention wherein a carbonaceous material, such as wood chips, are pryolyzed to produce a pyrolysis oil, which is then reformed to produce a syngas, which is then sent through various clean-up steps then to a methanation unit to produce synthetic natural gas.
  • a carbonaceous material such as wood chips
  • the present invention is directed to the production of synthetic natural gas (predominantly methane) from carbonaceous materials, preferably biomass materials.
  • Synthetic natural gas also sometimes called "green gas” is a renewable gas from biomass with natural gas specifications. Therefore, it can be transported through the existing gas infrastructure, substituting for natural gas in all existing applications.
  • Another advantage of green gas is that is carbon neutral. That is, using biomass as an energy supply will typically not result in a net CO 2 emission since its source can be replanted and uses CO 2 from the atmosphere during its growth period.
  • biomass feedstocks suitable for being converted in accordance with the present invention include trees such as red cedar, southern pine, hardwoods such as oak, cedar, maple and ash, as well as bagasse, rice hulls, rice straw, kennaf, old railroad ties, dried distiller grains, corn stalks and cobs and straw.
  • biomass feedstocks suitable for being converted in accordance with the present invention include trees such as red cedar, southern pine, hardwoods such as oak, cedar, maple and ash, as well as bagasse, rice hulls, rice straw, kennaf, old railroad ties, dried distiller grains, corn stalks and cobs and straw.
  • Cellulosic materials are the more preferred biomass feedstocks, with wood and dried distillers grains being the most preferred.
  • Biomass is typically comprised of three major components: cellulose, hemicellulose and lignin.
  • Cellulose is a straight and relatively stiff molecule with a polymerization degree of approximately 10,000 glucose units (Ce sugar).
  • Hemicellulose are polymers built of C 5 and C ⁇ sugars with a polymerization degree of about 200 glucose units. Both cellulose and hemicellulose can be vaporized with negligible char formation at temperatures above about 500 0 C.
  • lignin is a three dimensional branched polymer composed of phenolic units. Due to the aromatic content of lignin, it degrades slowly on heating and contributes to a major fraction of undesirable char formation.
  • biomass In addition to the major cell wall composition of cellulose, hemicellulose and lignin, biomass often contains varying amounts of species called "extractives". These extractives, which are soluble in polar or non-polar solvents, are comprised of terpenes, fatty acids, aromatic compounds and volatile oil. [0013] In most instances the carbonaceous mateials used in the practice of the present invention will be found in a form in which the particles are too large for conducting through the tubes of the pyrolysis unit. Thus, it will usually be necessary to grind the carbonaceous material to an effective size.
  • the carbonaceous material is ground, otherwise reduced in size, to a suitable size of about 1/32 inch to about 1 inch, preferably from about 1/16 inch to about Ms inch, and more preferably from about 1/8 inch to about 1/4 inch. Grinding techniques are well know and varied, thus any suitable grinding technique and equipment can be used for the particular carbonaceous material being converted.
  • the type of pyrolysis preferred for use in the practice of the present invention is known as "fast pyrolysis" which is a thermal decomposition process that occurs at moderate temperatures with a high heat transfer rate to the carbonaceous particles and a short hot vapor residence time in the reaction zone.
  • fast pyrolysis is a thermal decomposition process that occurs at moderate temperatures with a high heat transfer rate to the carbonaceous particles and a short hot vapor residence time in the reaction zone.
  • Several conventional reactor configurations have been used in the art, such as bubbling fluid beds, circulating and transported beds, vortex or cyclonic reactors, and ablative reactors. While all of these reactors have their advantages they are all faced with limitations, such as the tendency of fluid bed reactors to produce more gas and coke then the desired pyrolysis oil, the preferred pyrolysis product of the present invention.
  • the pyrolysis reactor of the present invention contains a plurality of vertically oriented straight tubes within the enclosed reactor vessel which is heated by use of a suitable heating device, such
  • the pyrolysis of biomass as practiced by the present invention produces a liquid product, pyrolysis oil or bio-oil that can be readily stored and transported.
  • Pyrolysis oil is a renewable liquid fuel can be used for production of chemicals and liquid fuels, or as herein for the production of synthetic natural gas.
  • synthetic natural gas is a very desirable product because it is derived from a renewable source and it can be used as a substitute for natural gas for all natural gas applications.
  • pyrolysis requires that a feedstock have less than about 15% moisture content, but there is an optimization between moisture content and conversion process efficiency. The actual moisture content will vary somewhat depending on the commercial process equipment used.
  • the biomass received for processing can have a moisture content from about 40 to 60% it will have to be dried before pyrolysis. Any conventional drying technique can be used as long as the moisture content is lowered to less than about 15% when mixed with the superheated steam. For example, passive drying during summer storage can reduce the moisture content to about 30% or less. Active silo drying can reduce the moisture content down to about 12%. Drying can be accomplished either by very simple means, such as near ambient, solar drying or by waste heat flows or by specifically designed dryers operated on location. Also, commercial dryers are available in many forms and most common are rotary kilns and shallow fluidized bed dryers.
  • the carbonaceous feedstock is conducted via line 10 and superheated steam is conducted via line 12 to mixing zone Mix wherein the two are sufficiently mixed before being conducted via line 14 into pyrolysis process unit P.
  • the superheated steam which will be at a temperature from about 315°C to about 700 0 C acts as both a source of hydrogen as well as a transport medium.
  • the amount of superheated steam to feedstock will be an effective amount. By effective amount we mean at least that amount needed to provide sufficient transport of the feedstock. That ratio of superheated steam to feedstock, on a volume to volume basis, will typically be from about 0.2 to 2.5, preferably from about 0.3 to 1.0.
  • the temperature conditions for the pyrolysis reaction will be described later in detail.
  • the steam is preferably introduced so that the feedstock is diluted to the point where it can easily be transported through the reactor tubes. Fluidization will typically result and can realize fluid pyrolysis by virtue of good contact among steam, feed polymers and heat decomposition products of carbonaceous material liberated in the gas phase.
  • the mixture of steam and feedstock which will be at a temperature of above its dew point of greater than about 230 0 C, is fed to the pyrolysis reactor P via line 14 into a flow divider FD where it is distributed into the plurality of vertically oriented straight reactor tubes of effective internal diameter and length within a metal cylindrical vessel of suitable size.
  • Flow divider FD can be any suitable design that will divide the feedstock substantially equally among the plurality of reactor tubes.
  • the reactor tubes for the pyrolysis reactor are straight instead of coiled because the residence time needs to be very short in order to produce the maximum amount of oil without the production of an undesirable amount of gas.
  • the temperature of the mixture entering the pyrolysis unit will be at least about 230 0 C.
  • Typical internal diameters for the pyrolysis reactor tubes will be from about 2 to about 4 inches, preferably from about 2.5 to about 3.5 inches, and more preferably about 3 inches.
  • the feedstock passing though the pyrolysis reactor tubes is subjected to fast pyrolysis at temperatures from about 400 0 C to about 650 0 C and pressures from about 3 to 35 psig, preferably from about 5 psig to about 35 psig.
  • the residence time of the feedstock in the pyrolysis reactor will be an effective residence time.
  • effective residence time we mean that amount of time that will result in the maximum yield of oil without excess gas make.
  • this effective amount of time for purposes of this invention will be from about 0.2 to about 7 seconds, preferably from about 0.3 seconds to about 5 seconds.
  • the heating rate will be a relatively high heating rate of about 1,000 0 C per second to about 10,000 0 C per second.
  • the high heating rate in the pyrolysis reactor of the present invention causes the liquid intermediate products of pyrolysis to condense before further reaction breaks down higher molecular weight species into gaseous products.
  • the high reaction rates also minimize char formation, and under preferred conditions substantially no char is formed.
  • the major products is gas, thus the need for the present process to operate at low enough temperatures to maximize the production of pyrolysis oils.
  • the source of heat for the pyrolysis unit, as well as the reformer of the present invention can be any suitable source, it is preferred that the source of heat be one or more burners B located at bottom of the pyrolysis and reforming process unit.
  • Fuel for the burners B can be any suitable fuel. It is preferred that at least a portion of the fuel to the burners be obtained from the present process itself, such as the syngas produced in either the pyrolysis reactor or in the reformer. For example at least a portion of syngas stream 20 can be diverted via line 21 and used as a fuel to burners B. A portion of the syngas stream 20 can also be combined with syngas stream of line 30.
  • Flue gas which will typically be comprised of CO 2 and N 2 is exhausted from the pyrolysis reactor via line 15 and the reaction products from the pyrolysis reactor are sent via line 16 to quench zone Q resulting in a mixture of liquid, gaseous and solid products. Most of the solids, which will typically be in the form of ash, will be collected from quench zone Q via line 17.
  • the liquid product will be in the form of a pyrolysis oil and the gaseous product will be a syngas.
  • the resulting liquid and gaseous products are conducted via line 18 to first separation zone Sl wherein a syngas stream is separated from the pyrolysis oil and collected overhead via line 20 or a portion being diverted via line 21 to either or both of burners B.
  • This syngas stream is comprised primarily of hydrogen, carbon dioxide, carbon monoxide, and methane.
  • the pyrolysis oil stream which may contain some remnants of char and ash formed during pyrolysis, is conducted via line 22 to reformer R along with an effective amount of superheated steam via line 23. It is preferred that reformer R contains a plurality of coiled reactor tubes within an enclosed reactor vessel heated by a suitable heating means, such as one or more .burners.
  • At least a portion of the pyrolysis oil is converted to syngas in reformer
  • the inlet temperature of the feedstock and superheated steam entering reformer R will preferably be about 200 0 C.
  • the exit temperature of the product syngas leaving reformer R via line 24 will typically be from about 850 0 C and 1200 0 C 5 preferably between about 900 0 C and about 1000 0 C.
  • Pressure in the reformer is not critical, but it will typically be at about 3 to 500 psig. Also, it is preferred that the residence time in the reformer be from about 0.4 to about 1.5 seconds.
  • heat recovery zone HRl where it is preferred that water be the heat exchange medium and that the water be passed as preheated steam to one or both of the pyrolysis reactor P or reformer R via lines 25 where it is further heated to produce at least a portion of the superheated steam used for both units.
  • Heat Recovery zone HRl can be any suitable heat exchange device, such as the shell-and-tube type wherein water is used to remove heat from product stream 24.
  • second separation zone S2 contains a gas filtering means and preferably a cyclone (not shown) and optionally a bag house (not shown) to remove at least a portion, preferably substantially all, of the remaining ash and other solid fines from the syngas.
  • the filtered solids are collected via line 28 for disposal.
  • the filtered syngas stream is then passed via line 30 to water wash zone
  • the water wash zone preferably comprises a column packed with conventional packing material, such as copper tubing, pall rings, metal mesh or other such materials.
  • the syngas passes upward countercurrent to down-flowing water which serves to further cool the syngas stream to about ambient temperature, and to remove any remaining ash that may not have been removed in second separation zone S2.
  • the water washed syngas stream is then passed via line 32 to oil wash zone OW where it is passed countercurrent to a down-flowing organic liquid stream to remove any organics present, such as benzene, toluene, xylene, or heavier hydrocarbon components via line 35 that may have been produced in the reformer.
  • the down- flowing organic stream will be any organic stream in which the organic material being removed is substantially soluble. It is preferred that the down-flowing organic stream be a hydrocarbon stream, more preferably a petroleum fraction.
  • the preferred petroleum fractions are those boiling in naphtha to distillate boiling range, more preferably a C ⁇ to C 20 hydrocarbon stream, most preferably a Qs hydrocarbon stream.
  • the resulting syngas stream is conducted via line 34 to acid gas scrubbing zone AGS wherein acidic gases, preferably CO 2 and H 2 S are removed.
  • acidic gases preferably CO 2 and H 2 S are removed.
  • Any suitable acid gas treating technology can be used in the practice of the present invention.
  • any suitable scrubbing agent preferably a basic solution can be used in the acid gas scrubbing zone AGS that will adsorb the desired level of acid gases from the vapor stream. It will be understood that it may be desirable to leave a certain amount of CO 2 in the scrubbed stream depending on the intended use of resulting methane product stream from the methanation unit. For example, if the methane product stream is to be introduced into a natural gas pipeline, no more than about 4 vol. % of CO 2 should be remain.
  • One suitable acid gas scrubbing technology is the use of an amine scrubber.
  • Non-limiting examples of such basic solutions are the amines, preferably diethanol amine, mono-ethanol amine, and the like. More preferred is diethanol amine.
  • Another preferred acid gas scrubbing technology is the so-called "Rectisol Wash” which uses an organic solvent, typically methanol, at subzero temperatures.
  • the scrubbed stream can also be passed through one or more guard beds (not shown) to remove catalyst poisoning impurities such as sulfur, halides etc.
  • the treated stream is passed via line 36 from acid gas scrubbing zone AGS to methanation zone M.
  • Methanation of syngas involves a reaction between carbon oxides, i.e. carbon monoxide and carbon dioxide, and hydrogen in the syngas to produce methane and water, as follows:
  • methanation zone M which is preferably comprised of two or more, more preferably three, reactors each containing a suitable methanation catalyst.
  • the methanation reaction is strongly exothermic. Generally, the temperature increase in a typical methanator gas composition is about 74°C for each 1% of carbon monoxide converted and 60 0 C for each 1% carbon dioxide converted. Because of the exothermic nature of methanation reactions (1) and (2), the temperature in the methanation reactor during methanation of syngas has to be controlled to prevent overheating of the reactor catalyst. Also high temperatures are undesirable from an equilibrium standpoint and reduce the amount of conversion of syngas to methane since methane formation is favored at lower temperatures. Formation of soot on the catalyst is also a concern and may require the addition of water to the syngas feedstock.
  • methanation zone M preferably comprises a series of three adiabatic methanation reactors Rl, R2 and R3. Each of these reactors is configured to react carbon oxide and hydrogen contained in the syngas in the presence of a suitable catalyst to produce methane and water, in accordance with the reactions (1) and (2) set forth hereinabove.
  • Each of the methanation reactors includes a catalyst capable of promoting methanation reactions between carbon oxides and hydrogen in the syngas feedstock.
  • Any conventional methanation catalyst is suitable for use in the practice of the present invention, although nickel catalysts are most commonly used and the more preferred for this invention. Such catalysts are, especially those containing greater than 50% nickel, are generally stable against thermal and chemical sintering during methanation of undiluted syngas streams. Alternatively, other stable catalysts that are active and selective towards methane may be used in the methanation reactors.
  • heat recover zones HR2 and HR3 are used to remove heat from the stream as it passed from reactor Rl to reactor R2 and reactor R2 to reactor R3 respectively.
  • Any suitable exchange device can be used, preferably a shell-and-tube type wherein water can be used to remove heat from the product stream. The water can then be recycled to one or both of 12 and 23 where it can be further heated to produce superheated steam.
  • the inlet and outlet temperatures of the streams entering and exiting methanation reactors Rl - R3 can be controlled by varying the percentage of syngas being delivered to each of the reactors as well as how much heat is exchanged by heat exchangers HR2 and HR3.
  • the inlet temperature of reactors Rl and R2 will be from about 400 0 F to about 450 0 F with an outlet temperature of about 500 0 F to about 800 0 F.
  • the third reactor, which will operate at a lower temperature than that of reactors Rl and R2 will have an inlet temperature of about 400 0 F and an outlet temperature of about 500 0 F.
  • the step of recovering at least a part of generated heat and/or at least a part of waste heat in the regeneration zone and effectively utilizing the recovered heat is further provided.
  • the recovered heat can be effectively utilized, for example, for drying and heating of the biomass feedstock and the generation of steam as the gasifying agent.
  • the product stream from the methanation unit will be comprised predominantly of methane. That is, it will contain at least about 75 vol.%, preferably at least about 85 vol.%, and more preferably at least about 95 vol.% methane. If the methane product stream is to be introduced into a natural gas pipeline, then it must meet the specification requirements for the pipeline.
  • the product methane stream is preferably introduced into a natural gas pipeline and utilized at any downstream facility.
  • One such facility if preferably a plant that converts the methane to syngas then to other products, such as alcohols, transportation fuels, or lubricant base stocks.
  • any suitable process can be used that convert methane or natural gas to syngas.
  • Preferred methods include steam reforming and partial oxidation. More preferred is steam reforming. Steam reforming of methane is a highly endothermic process and involves following reactions:
  • the steam reformer will preferably be one similar to reformer R hereof, which is a coiled tubular reactor.
  • Preferred steam reforming catalysts are nickel containing catalysts, particularly nickel (with or without other elements) supported on alumina or other refractory materials, in the above catalytic processes for conversion of methane (or natural gas) to syngas is also well known in the prior art. Kirk and Othmer, Encyclopedia of Chemical Technology, 3rd Ed., 1990, vol. 12, p. 951; Ullmann's Encyclopedia of Industrial Chemistry, 5th Ed., 1989, vol. A12, pp. 186 and 202; U.S. Pat. No. 2,942,958 (1960); U.S. Pat. No. 4,877,550 (1989); U.S.
  • the catalytic steam reforming of methane, or natural gas, to syngas is a well established technology practiced for commercial production of hydrogen, carbon monoxide and syngas (i.e., a mixture of hydrogen and carbon monoxide).
  • hydrocarbon feed is converted to a mixture Of H 2 , CO and CO 2 by reacting hydrocarbons with steam over a supported nickel catalyst such as NiO supported on alumina at elevated temperature (850 0 C to 1000 0 C) and pressure (10-40 arm) and at steam to carbon mole ratio of 2-5 and gas hourly space velocity of about 5000-8000 per hour.

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Abstract

L'invention concerne la production de gaz naturel de synthèse à partir d'une matière carbonée, de préférence à partir d'une matière de type biomasse telle que le bois. Ladite matière carbonée est préalablement pyrolysée, puis soumise à un processus de reformage à la vapeur pour produire un gaz de synthèse qui subit ensuite plusieurs étapes d'épuration avant d'être introduit dans une zone de méthanation pour générer un gaz naturel de synthèse.
PCT/US2007/016616 2006-07-24 2007-07-24 Conversion de matières carbonées en gaz naturel de synthèse par pyrolyse, reformage et méthanation WO2008013794A2 (fr)

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WO2013102340A1 (fr) * 2012-01-06 2013-07-11 Kong Lingzeng Procédé et dispositif de préparation de gaz
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CN104152166B (zh) * 2014-06-11 2016-05-04 华南理工大学 一种油页岩炼油集成伴生煤气化制氢综合利用系统及工艺
GB2539518A (en) * 2015-06-16 2016-12-21 Sage & Time Llp A gasification system
GB2539518B (en) * 2015-06-16 2017-09-13 Sage & Time Llp System for pyrolysis and gasification
CN108998097A (zh) * 2018-08-28 2018-12-14 朋仁锋 一种煤气化方法
US20230203382A1 (en) * 2020-05-08 2023-06-29 Basf Se Process for purifying a crude pyrolysis oil originating from the pyrolysis of plastic waste

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