WO2019206451A1 - Production d'un produit gazeux contenant au moins du monoxyde de carbone - Google Patents

Production d'un produit gazeux contenant au moins du monoxyde de carbone Download PDF

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Publication number
WO2019206451A1
WO2019206451A1 PCT/EP2019/025094 EP2019025094W WO2019206451A1 WO 2019206451 A1 WO2019206451 A1 WO 2019206451A1 EP 2019025094 W EP2019025094 W EP 2019025094W WO 2019206451 A1 WO2019206451 A1 WO 2019206451A1
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WO
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Prior art keywords
carbon dioxide
electrolysis
temperature
low
heat
Prior art date
Application number
PCT/EP2019/025094
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German (de)
English (en)
Inventor
Andreas Peschel
Benjamin HENTSCHEL
Original Assignee
Linde Aktiengesellschaft
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
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Publication of WO2019206451A1 publication Critical patent/WO2019206451A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C25B1/01—Products
    • C25B1/02—Hydrogen or oxygen
    • C25B1/04—Hydrogen or oxygen by electrolysis of water
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B15/00—Operating or servicing cells
    • C25B15/08—Supplying or removing reactants or electrolytes; Regeneration of electrolytes
    • 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
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C20/00—Capture or disposal of greenhouse gases
    • Y02C20/40—Capture or disposal of greenhouse gases of CO2
    • 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
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
    • 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
    • Y02P20/10—Process efficiency
    • Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines

Definitions

  • the present invention relates to a process for producing a gas product containing at least carbon monoxide and a corresponding plant according to the respective preambles of the independent claims.
  • Synthesis gas is a predominantly or exclusively carbon monoxide and hydrogen-containing gas mixture. Synthesis gas is currently produced by various methods, e.g. by steam reforming of natural gas or by
  • Hydrogen can also be produced by means of water electrolysis (for example by means of alkaline electrolysis or using a proton exchange membrane).
  • the production of carbon monoxide is by means of high-temperature electrolysis of
  • Carbon dioxide possible as disclosed for example in WO 2013/131778 A2.
  • a synthesis gas can also be obtained.
  • Proton exchange membrane (English: Proton Exchange Membrane, PEM) can be used. In this case, the following cathode reactions take place:
  • the protons or other corresponding charge carriers are selectively transferred via a membrane from the anode to the cathode side.
  • the respective formation reactions compete at the cathode, resulting in synthesis gases with different hydrogen / carbon monoxide ratios.
  • other products of value may also be formed in the low-temperature co-electrolysis.
  • HT high temperature
  • SOEC solid oxide electrolysis cells
  • the oxygen ions are in this case conducted essentially selectively via a ceramic membrane from the anode to the cathode. It is not fully understood whether the reaction proceeds according to reaction equation 4 in the manner shown. It is also possible that only hydrogen is formed electrochemically and carbon monoxide forms according to the reverse water gas shift reaction in the presence of carbon dioxide: C0 2 + H 2 H 2 0 + CO (7)
  • the gas mixture formed in the high-temperature co-electrolysis is in the water gas shift equilibrium (or close to this).
  • the concrete nature of the formation of carbon monoxide has no influence on the present invention.
  • the present invention has as its object to provide improved measures for the production of carbon monoxide or synthesis gas using an electrolysis, in particular a low-temperature (co-) electrolysis.
  • the present invention proposes a method for
  • At least carbon monoxide-containing gas product is here in particular carbon monoxide different purities or synthesis gas or a comparable gas mixture, ie a gas mixture containing not only carbon monoxide but also significant amounts of hydrogen understood.
  • the at least carbon monoxide-containing gas product is the at least carbon monoxide-containing gas product
  • the molar ratio of hydrogen to carbon monoxide in the gas product can in particular in a range of 1: 10 to 10: 1, 2: 8 to 8: 2 or 4: 6 to 6: 4, wherein the molar fraction of hydrogen and carbon dioxide together exceed 50%, 60%, 70%, 80 %, 90%, 95% or 99% can be and any remaining remainder may be formed in particular from carbon dioxide or inert gases such as nitrogen or noble gases of the air.
  • the molar ratio of hydrogen to carbon monoxide in the gas product may be in particular about 1 or about 2 or about 3, the stoichiometry number in particular at about 2.
  • the gas product is correspondingly poor or free of hydrogen, ie it is a carbon monoxide-rich gas product or pure carbon monoxide.
  • streams, gas mixtures, etc. as used herein may be rich or poor in one or more components, with the term “rich” being for a content of at least 50%, 60%, 75%, 80%, 90%, 95%, 98%, 99%, 99.5%, 99.9% or 99.99% and the statement "poor” for a maximum content of 50%, 40%, 25%, 20%, 10%, 5%, 2 %, 1%, 0.5%, 0.1% or 0.01% on molar, weight or
  • volume base can stand. If more than one component is specified, the term “rich” or “poor” refers to the sum of all components. If, for example, “carbon monoxide” is mentioned here, it can be a pure gas or a mixture rich in carbon monoxide. A gas mixture containing "predominantly" one or more components is particularly rich in this or this in the sense explained.
  • Material streams, gas mixtures, etc. may also be “enriched” or “depleted” in one or more components as used herein, which terms refer to a content in a starting mixture. They are “enriched” if they are at least 1, 1, 5, 1, 5, 2, 5, 10, 100, or 1, 000 times, “depleted,” if at most 0.9 times, 0.75 times, 0.5 times, 0.1 times, 0.01 times or 0.001 times the content of one or more components, based on the
  • waste heat from a low-temperature electrolysis which can be formed as co-electrolysis of carbon dioxide and water, as explained above or as pure carbon dioxide electrolysis, and which is at least subjected to carbon dioxide to obtain carbon monoxide a heat pump to one or more further process steps to transfer.
  • Low-temperature electrolysis can be used advantageously.
  • heat is dissipated in particular by means of air coolers or cooling water and discharged from the system.
  • the heat pump used in the context of the present invention may be formed in a fundamentally known manner and operated by means of one or more of the working medium also specified below.
  • the or the working fluid is or will be particularly at low pressure, i. at a lower pressure level, vaporized by the heat of low-temperature electrolysis.
  • the working fluid (s) will then be or will be pressurized to one of greater pressure, i. E., By one or more compressors. to an upper pressure level, compressed. Subsequently, or will the or the work equipment on the upper
  • methanol used is the lower pressure level at about 2 bar abs. and the upper pressure level at about 6 bar abs.
  • 1 kW of heat are removed from the low-temperature electrolysis and to the one or more downstream
  • the compression to the upper pressure level here is about 0.15 kW, and as a further cooling capacity for the condensation of methanol evaporating in the expansion to the lower pressure level about 0.15 kW as additional cooling capacity, for example in an air cooler needed.
  • additional cooling capacity for example in an air cooler needed.
  • the present invention proposes a method for producing a gas product comprising at least carbon monoxide, in which an electrolysis insert comprising at least carbon dioxide is formed and subjected to low-temperature electrolysis to obtain a crude gas containing at least carbon monoxide and carbon dioxide, the electrolysis insert comprising at least part of a carbon dioxide containing starting mixture using a first
  • Carbon dioxide separation is formed and / or the gas product is formed from at least a portion of the raw gas using a second carbon dioxide separation.
  • the electrolysis insert may in particular also contain other components, depending on the process conditions, in particular water, but it may also consist predominantly or exclusively of carbon dioxide. Accordingly, the raw gas may include various other components, in the case of
  • Corresponding further components can also be separated off.
  • the carbon dioxide removal can be subjected to a portion of the raw gas even after a corresponding separation of other components such as water.
  • the second separation of carbon dioxide used in the formation of the gas product can in particular also be used to form a fraction containing carbon dioxide, which in turn is at least partly used in the formation of the electrolysis insert can be used. In other words, this can be separated
  • Carbon dioxide be recycled in the process of the present invention.
  • Kohldioxidabtrennung comprise a laundry in which a washing liquid loaded with carbon dioxide and by expelling the carbon dioxide by means of
  • washing liquid supplied regeneration heat is regenerated.
  • Corresponding washes are known in principle from the prior art. Reference is made to the relevant literature.
  • a fluid to be processed in the present case the raw gas or a gas mixture formed using a part of the raw gas, is brought into contact with a washing liquid of suitable type. This is typically done in a corresponding column with suitable internals.
  • the washing liquid is chosen so that the component contained in the fluid to be separated, in this case carbon dioxide, dissolves or binds as much as possible in the washing liquid.
  • Washing liquid can be regenerated by heating it in another apparatus, in particular another column, whereby the dissolved or bound component is expelled.
  • the heat used in this context is referred to herein as "regeneration heat". It is provided in the context of the present invention, in particular by means of the heat pump using waste heat of low-temperature electrolysis. The achievable temperature level is particularly suitable for a corresponding use.
  • a so-called direct air capture ie a direct removal of carbon dioxide can be made. This is an adsorption or a mixture of adsorption and absorption, wherein a liquid absorbent is applied to a solid and is held there by adhesion and / or cohesive forces.
  • Corresponding combined separation principle is not limited to the classic direct air capture but can be used in the context of the present invention in other context. Again, there is a regeneration with heat, so “regeneration heat” as already explained above.
  • regeneration heat in addition to the typical for direct air capture amines as adsorbents and ionic liquids can be used in the present invention.
  • any procedure is also on relevant literature, for example, to the publication "Direct Air Capture of C0 2 with Chemicals, a technology assessment for the Panel on Public Affairs" of the American Physical Society from the first June 2011 referenced.
  • the first and / or the second carbon dioxide separation comprises an adsorption in which an adsorbent is charged with carbon dioxide and regenerated by desorbing the carbon dioxide by means of regeneration heat supplied by the adsorbent.
  • an adsorbent is charged with carbon dioxide and regenerated by desorbing the carbon dioxide by means of regeneration heat supplied by the adsorbent.
  • Temperature change adsorption are used.
  • a combination of adsorption and absorption can also take place, as mentioned above with reference to the example of direct air capture.
  • the temperature swing adsorption takes advantage of the temperature dependence of adsorption processes.
  • An adsorbent that is in a suitable
  • Adsorber essenceer is housed, is thereby flows in an operating cycle at a lower temperature level with the gas mixture stream to be separated and in this case with the or each separated components from the
  • the adsorbent can then be largely freed by heating, ie introducing thermal energy, from this or these components and regenerated in this way.
  • at least two adsorption units are required for continuous operation of a temperature change adsorption system, so that one of the
  • Adsorption with the gas mixture stream to be separated flows through and thus can be used to separate the gas mixture stream. This too can be done within the scope of the present invention.
  • the heat used in this context is referred to here as "regeneration heat”. It can also be provided in the context of the present invention, in particular by means of the heat pump using waste heat of low-temperature electrolysis. The achievable temperature level is also particularly suitable for use in an adsorptive process as explained.
  • Regeneration heat for absorptive or adsorptive carbon dioxide removal at least part of the heat pump from the
  • a laundry which can be used in the context of the present invention in the first and / or in the second carbon dioxide removal, can, as already mentioned, be carried out in particular in the form of a chemical and / or a physical wash.
  • a chemical washing a binding of a component contained in the washing liquid with the component to be separated takes place, here carbon dioxide.
  • a physical wash is a purely physical absorption without chemical bonding.
  • the washing can be carried out in particular by using one or more compounds which consist of inorganic carbonates, amines, alcohols (in particular methanol), one or more organic methyl or ethyl esters (in particular methyl or ethyl acetate), one or more organic compounds Methyl or ethyl ethers (especially dimethyl ether), polyethylene glycol, acetone, acetonitrile, n-methylpyrrolidone, dimethylformamide or Acetonitrile are selected.
  • particular preference may be given to using selexol, Genosorb and / or purisol processes as the laundry process.
  • the low-temperature electrolysis can be carried out in particular at an electrolysis temperature level which is 20 to 100 ° C., in particular 40 to 80 ° C.
  • a low-temperature electrolysis is operated at appropriate temperature levels, in particular with an efficiency of 30 to 80%, in particular 40 to 70%. This entails that typically 20 to 70%, in particular 30 to 60% of the power used must be dissipated as waste heat.
  • the heat pump in the context of the present invention, this comparatively large amount of waste heat, but for use in other process steps initially on an unsuitable
  • the waste heat of the low-temperature electrolysis is advantageously transferred using the heat pump by means of one or more working medium flows at one or more temperature levels above the electrolysis temperature level.
  • Increase in temperature can be done in particular by 20 to 100 K, more particularly by 30 to 50 K, for example by about 40 K.
  • Sorption heat pumps differ from compression heat pumps in that one or more working fluids are not or will be compressed by a mechanical compressor. Instead, a so-called thermal compressor is used. Sorption heat pumps work like
  • Compression heat pumps based on a cycle process.
  • heat is used for compression Sorption heat pump can operate on the basic principles of absorption and adsorption and are also referred to as absorption or Adsorptions Scripumpen.
  • a working fluid for example water
  • the so-called solvent for example lithium bromide
  • ammonia can be used as a working fluid and water as a solvent.
  • Absorption heat exchangers have the particular advantage that only comparatively little additional (electrical) energy is needed for their operation, essentially for a solvent pump, which transports a solvent-solvent mixture from the evaporator to the expeller.
  • an adsorption heat pump relies on the interaction between adsorption and desorption on a porous solid (adsorbent), such as silica gel or zeolite.
  • adsorbent such as silica gel or zeolite.
  • working fluid for example, water
  • Adsorption heat pump is essentially only energy needed for the transport of the working fluid, but not for compression.
  • the fluid stream or streams may or may be formed using, in particular, one or more working fluids comprising or comprising at least one hydrocarbon and / or at least one alcohol, for example methanol or ethanol.
  • one or more working fluids comprising or comprising at least one hydrocarbon and / or at least one alcohol, for example methanol or ethanol.
  • propane, butane and / or dimethyl ether are suitable as hydrocarbons.
  • Corresponding hydrocarbons can be used in heat pumps in the temperature ranges in question here.
  • Heat pumps operated with appropriate non-aqueous working fluids are also referred to as Organic Rankine Cycle (ORC) processes.
  • ORC Organic Rankine Cycle
  • corresponding waste heat alternatively or in addition to use in carbon dioxide removal, as mentioned several times, may also be associated with the process in one or more other
  • Process steps are used.
  • the further method step (s) may be used in particular for the further processing of at least part of the
  • Gas product can be used.
  • the method step (s) assigned to the method may in particular comprise one or more constituent chemical synthesis reactions or separation steps, the corresponding ones
  • Synthesis reactions downstream include. These include, for example, the synthesis of oxygenates, such as methanol; Ethanol, dimethyl ether, dimethylformamide, dimethyl carbonate, polyoxymethylene dimethyl ether, formaldehyde,
  • Methyl methacrylate formic, acetic and propionic acid.
  • corresponding synthetic reactions may include the generation of long chain alkenes and alkanes as well as typical Fischer-Tropsch products such as kersoin, gasoline, and waxes.
  • a preparation of phosgene or polycarbonates may be provided.
  • the synthesis reaction (s) may in particular comprise a hydroformylation and / or a synthesis of at least one further alcohol. Hydroformylation is also referred to as oxo synthesis and more rarely as Roelen synthesis or Roelen reaction. It is a homogeneously catalyzed reaction of olefins with carbon monoxide and hydrogen to produce aldehydes.
  • alcohols such as n-butanol can be formed.
  • organometallic cobalt or rhodium compounds can be used as hydroformylation catalysts.
  • the hydroformylation is typically carried out at pressures of about 10 bar to 100 bar and temperatures between 40 and 200 ° C.
  • the invention also extends to a plant for producing a gas product containing at least carbon monoxide, comprising means adapted to form an electrolysis insert containing at least carbon dioxide and means adapted to use the electrolysis insert to obtain a raw gas containing at least carbon monoxide and carbon dioxide subject to a low-temperature electrolysis, wherein means are provided which are adapted to form the Elektrolyse junk of at least a portion of a carbon dioxide-containing starting mixture using a first carbon dioxide separation and / or the gas product of at least a portion of the raw gas using a second carbon dioxide separation to build.
  • the plant is characterized in that means are provided which comprise a heat pump and which are adapted to dissipate waste heat from the low-temperature electrolysis using the heat pump and at least partially to the first and / or the second carbon dioxide separation and / or to transfer to at least one further method step assigned to the method.
  • FIG. 1 illustrates a system according to an embodiment of the invention in a schematic representation. Detailed description of the drawings
  • FIG. 1 illustrates a plant according to a particularly preferred embodiment of the invention and designated 100 as a whole.
  • the central component of the system 100 is an arrangement 10 for carrying out a low-pressure co-electrolysis of the type described above. This is fed to a feed stream A which contains at least carbon dioxide and possibly also water. Optionally, separately from the arrangement 10 for carrying out the low-pressure co-electrolysis supplied water is not illustrated separately in Figure 1.
  • a raw gas stream B is carried out, which contains in particular carbon monoxide and unreacted carbon dioxide of the feed stream A.
  • the crude gas stream B may in particular also contain hydrogen and water.
  • the crude gas stream B is fed to an arrangement 20 for carbon dioxide separation.
  • the carbon dioxide separation assembly 20 may be adapted for adsorptive or absorptive carbon dioxide removal, as is well known in the art.
  • absorptive removal may be in particular an amine and / or Laugeskysky
  • the adsorptive removal can be carried out using a suitable adsorbent material. From the arrangement 20 for carbon dioxide separation can in particular a
  • C product stream are carried out predominantly or exclusively
  • Carbon monoxide or carbon monoxide and hydrogen may contain. Furthermore, a carbon dioxide-rich stream D can be discharged from the arrangement 20 and returned to the arrangement 10 for carrying out the low-pressure co-electrolysis.
  • a further device 30 for separating off carbon dioxide to which is supplied a carbon dioxide-containing output stream E, for example a flue gas stream.
  • the further arrangement 30 for separating off carbon dioxide can likewise be designed for the adsorptive and / or absorptive removal of carbon dioxide.
  • a heat pump 40 which can be operated using a suitable working medium in the means 20 for carbon dioxide separation and / or the further means 30 for Carbon dioxide separation are transferred, as illustrated with G and H.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Gas Separation By Absorption (AREA)

Abstract

L'invention concerne un procédé de production d'un produit gazeux contenant au moins du monoxyde de carbone, selon lequel une charge d'électrolyse contenant au moins du dioxyde de carbone est formée et soumise à une électrolyse à basse température pour obtenir un gaz brut contenant au moins du monoxyde de carbone et du dioxyde de carbone, la charge d'électrolyse étant formée à partir d'au moins une partie d'un mélange de départ contenant du dioxyde de carbone par l'intermédiaire d'une première séparation de dioxyde de carbone et/ou le produit gazeux étant formé à partir d'au moins une partie du gaz brut par l'intermédiaire d'une deuxième séparation de dioxyde de carbone. Selon l'invention, la chaleur perdue de l'électrolyse à basse température est évacuée de l'électrolyse à basse température au moyen d'une pompe à chaleur et transférée au moins en partie à la première et/ou à la deuxième séparation de dioxyde de carbone. La présente invention concerne également une installation (100) correspondante.
PCT/EP2019/025094 2018-04-24 2019-04-02 Production d'un produit gazeux contenant au moins du monoxyde de carbone WO2019206451A1 (fr)

Applications Claiming Priority (2)

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DE102018003342.3 2018-04-24
DE102018003342.3A DE102018003342A1 (de) 2018-04-24 2018-04-24 Herstellung eines zumindest Kohlenmonoxid enthaltenden Gasprodukts

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WO2019206451A1 true WO2019206451A1 (fr) 2019-10-31

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Publication number Priority date Publication date Assignee Title
DE102019215620A1 (de) * 2019-10-11 2021-04-15 Siemens Aktiengesellschaft Verfahren und Vorrichtung zur Herstellung eines Produktgemischs mit einem kohlenstoffhaltigen Brennstoff

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WO2014154253A1 (fr) 2013-03-26 2014-10-02 Haldor Topsøe A/S Procédé de production de co à partir de co2 dans une cellule d'électrolyse à oxyde solide
WO2015014527A1 (fr) 2013-07-30 2015-02-05 Haldor Topsøe A/S Processus de production de co à haute pureté par purification par membrane du co produit par une pile à électrolyse à oxyde solide (soec)
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EP2940773A1 (fr) 2014-04-29 2015-11-04 Haldor Topsøe A/S Éjecteur pour système d'empilement de cellule d'électrolyse d'oxyde solide
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