WO2001010773A1 - Compact reactor - Google Patents
Compact reactor Download PDFInfo
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- WO2001010773A1 WO2001010773A1 PCT/GB2000/002887 GB0002887W WO0110773A1 WO 2001010773 A1 WO2001010773 A1 WO 2001010773A1 GB 0002887 W GB0002887 W GB 0002887W WO 0110773 A1 WO0110773 A1 WO 0110773A1
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- 238000006243 chemical reaction Methods 0.000 claims abstract description 32
- 238000009792 diffusion process Methods 0.000 claims abstract description 18
- 238000012546 transfer Methods 0.000 claims abstract description 13
- 239000003054 catalyst Substances 0.000 claims description 45
- 239000000446 fuel Substances 0.000 claims description 38
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 15
- 239000001257 hydrogen Substances 0.000 claims description 15
- 229910052739 hydrogen Inorganic materials 0.000 claims description 15
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 10
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 9
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 9
- 239000002245 particle Substances 0.000 claims description 7
- 229910052763 palladium Inorganic materials 0.000 claims description 6
- 229910052697 platinum Inorganic materials 0.000 claims description 5
- 229910052759 nickel Inorganic materials 0.000 claims description 4
- 229910052707 ruthenium Inorganic materials 0.000 claims description 4
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims 1
- 239000001301 oxygen Substances 0.000 claims 1
- 229910052760 oxygen Inorganic materials 0.000 claims 1
- 238000002485 combustion reaction Methods 0.000 description 30
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 22
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 14
- 238000002407 reforming Methods 0.000 description 11
- 238000000629 steam reforming Methods 0.000 description 10
- 229910052751 metal Inorganic materials 0.000 description 9
- 239000002184 metal Substances 0.000 description 9
- 239000012530 fluid Substances 0.000 description 7
- 239000002737 fuel gas Substances 0.000 description 7
- 230000000694 effects Effects 0.000 description 6
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- 238000013461 design Methods 0.000 description 4
- 229910052799 carbon Inorganic materials 0.000 description 3
- 150000002739 metals Chemical class 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 150000002815 nickel Chemical class 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- 239000000956 alloy Substances 0.000 description 2
- 229910045601 alloy Inorganic materials 0.000 description 2
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- 229930195733 hydrocarbon Natural products 0.000 description 2
- 150000002430 hydrocarbons Chemical class 0.000 description 2
- 229910052741 iridium Inorganic materials 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 238000006057 reforming reaction Methods 0.000 description 2
- 229910052703 rhodium Inorganic materials 0.000 description 2
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- 239000011949 solid catalyst Substances 0.000 description 2
- 239000003381 stabilizer Substances 0.000 description 2
- 239000010409 thin film Substances 0.000 description 2
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical class [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- 241000640882 Condea Species 0.000 description 1
- 229910000599 Cr alloy Inorganic materials 0.000 description 1
- 241000196324 Embryophyta Species 0.000 description 1
- 229910002651 NO3 Inorganic materials 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 239000005864 Sulphur Substances 0.000 description 1
- 206010042618 Surgical procedure repeated Diseases 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910002090 carbon oxide Inorganic materials 0.000 description 1
- 238000007084 catalytic combustion reaction Methods 0.000 description 1
- 238000001193 catalytic steam reforming Methods 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 1
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000000788 chromium alloy Substances 0.000 description 1
- UPHIPHFJVNKLMR-UHFFFAOYSA-N chromium iron Chemical compound [Cr].[Fe] UPHIPHFJVNKLMR-UHFFFAOYSA-N 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 229910052593 corundum Inorganic materials 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
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- 238000010586 diagram Methods 0.000 description 1
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- 238000009472 formulation Methods 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- DTZRLFJKQHIVQA-UHFFFAOYSA-N palladium(2+);dinitrate;hydrate Chemical compound O.[Pd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O DTZRLFJKQHIVQA-UHFFFAOYSA-N 0.000 description 1
- GPNDARIEYHPYAY-UHFFFAOYSA-N palladium(ii) nitrate Chemical compound [Pd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O GPNDARIEYHPYAY-UHFFFAOYSA-N 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- 150000003303 ruthenium Chemical class 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000013341 scale-up Methods 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 238000003980 solgel method Methods 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 230000009974 thixotropic effect Effects 0.000 description 1
- 229910001845 yogo sapphire Inorganic materials 0.000 description 1
Classifications
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28F—DETAILS OF HEAT-EXCHANGE AND HEAT-TRANSFER APPARATUS, OF GENERAL APPLICATION
- F28F13/00—Arrangements for modifying heat-transfer, e.g. increasing, decreasing
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/24—Stationary reactors without moving elements inside
- B01J19/2475—Membrane reactors
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/44—Palladium
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/74—Iron group metals
- B01J23/755—Nickel
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
- B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/0215—Coating
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/0215—Coating
- B01J37/0225—Coating of metal substrates
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/008—Details of the reactor or of the particulate material; Processes to increase or to retard the rate of reaction
- B01J8/009—Membranes, e.g. feeding or removing reactants or products to or from the catalyst bed through a membrane
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
- B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
- B01J8/06—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds in tube reactors; the solid particles being arranged in tubes
- B01J8/067—Heating or cooling the reactor
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
- C01B3/384—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts the catalyst being continuously externally heated
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28D—HEAT-EXCHANGE APPARATUS, NOT PROVIDED FOR IN ANOTHER SUBCLASS, IN WHICH THE HEAT-EXCHANGE MEDIA DO NOT COME INTO DIRECT CONTACT
- F28D7/00—Heat-exchange apparatus having stationary tubular conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall
- F28D7/0008—Heat-exchange apparatus having stationary tubular conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall the conduits for one medium being in heat conductive contact with the conduits for the other medium
- F28D7/0025—Heat-exchange apparatus having stationary tubular conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall the conduits for one medium being in heat conductive contact with the conduits for the other medium the conduits for one medium or the conduits for both media being flat tubes or arrays of tubes
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
- B01J2208/00008—Controlling the process
- B01J2208/00017—Controlling the temperature
- B01J2208/00106—Controlling the temperature by indirect heat exchange
- B01J2208/00309—Controlling the temperature by indirect heat exchange with two or more reactions in heat exchange with each other, such as an endothermic reaction in heat exchange with an exothermic reaction
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
- B01J2208/00008—Controlling the process
- B01J2208/00548—Flow
- B01J2208/00557—Flow controlling the residence time inside the reactor vessel
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/00049—Controlling or regulating processes
- B01J2219/00051—Controlling the temperature
- B01J2219/00074—Controlling the temperature by indirect heating or cooling employing heat exchange fluids
- B01J2219/00087—Controlling the temperature by indirect heating or cooling employing heat exchange fluids with heat exchange elements outside the reactor
- B01J2219/00103—Controlling the temperature by indirect heating or cooling employing heat exchange fluids with heat exchange elements outside the reactor in a heat exchanger separate from the reactor
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/00049—Controlling or regulating processes
- B01J2219/00051—Controlling the temperature
- B01J2219/00074—Controlling the temperature by indirect heating or cooling employing heat exchange fluids
- B01J2219/00117—Controlling the temperature by indirect heating or cooling employing heat exchange fluids with two or more reactions in heat exchange with each other, such as an endothermic reaction in heat exchange with an exothermic reaction
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/00049—Controlling or regulating processes
- B01J2219/00164—Controlling or regulating processes controlling the flow
- B01J2219/00166—Controlling or regulating processes controlling the flow controlling the residence time inside the reactor vessel
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/19—Details relating to the geometry of the reactor
- B01J2219/192—Details relating to the geometry of the reactor polygonal
- B01J2219/1923—Details relating to the geometry of the reactor polygonal square or square-derived
- B01J2219/1925—Details relating to the geometry of the reactor polygonal square or square-derived prismatic
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/08—Methods of heating or cooling
- C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
- C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F28—HEAT EXCHANGE IN GENERAL
- F28F—DETAILS OF HEAT-EXCHANGE AND HEAT-TRANSFER APPARATUS, OF GENERAL APPLICATION
- F28F2255/00—Heat exchanger elements made of materials having special features or resulting from particular manufacturing processes
- F28F2255/18—Heat exchanger elements made of materials having special features or resulting from particular manufacturing processes sintered
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- 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
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
Definitions
- the present invention relates to a reactor assembly having a first region for performing an endothermic reaction and a second region for performing an exothermic reaction and the reactor assembly being arranged to provide good heat conduction between the first and second regions.
- the reactor assembly is particularly suitable for use as a steam reformer in which the endothermic catalytic conversion of steam and a fuel stream into hydrogen and carbon oxides is performed in the first region and the exothermic combustion of a fuel stream is performed in the second region.
- Hydrogen produced by a steam reformer is particularly suitable for use in one or more fuel cells to produce electricity.
- a reactor designed for steam reforming of hydrocarbon fuel comprises a first reaction chamber to perform the catalytic steam reforming reaction within which solid catalyst particles are disposed.
- the first reaction chamber is in a good heat conducting relationship with a second reaction chamber which may be a furnace surrounding the first reaction chamber to provide heat to the first reaction chamber to make the steam reforming reaction more energetically favourable.
- a reactor is disclosed in US 4203950.
- Another type of steam reformer is a Haldor Topsoe Heat Exchange Reformer as described in 'Scale up Study of Heat Exchange Reformer for 5MW Fuel Cell Plant' from the 1992 Fuel Cell Seminar Proceedings, Courtesy Associates Inc., Washington DC, USA.
- This reformer has a toroidal shaped catalyst bed acting as the first reaction chamber with heat from a burner supplied to the inside and outside of the toroid. The application of heat to both the inside and outside of the toroidal shaped catalyst bed improves the heat transfer to the first reaction chamber and so also the energy density of the reformer when used to supply hydrogen to a fuel cell.
- a further type of steam reformer is an IHI plate reformer as described in EP-A-0430184.
- This reformer includes a multi-layer unit comprised of parallel plates that are welded together to form a series of chambers. Alternating chambers are used for steam reforming and for combustion which improves the heat transfer between the combustion region and the steam reforming region and so also the energy density of this type of reformer when used with a fuel cell.
- reactors are generally large and heavy because of their need to house solid catalyst particles and/or because of their brazed or welded construction.
- the reactors are particularly unsuitable for use in mobile applications such as to provide hydrogen to one or more fuel cells in a vehicle. Furthermore it is desirable to improve the heat transfer between the first and second regions of such reactors.
- a reactor assembly comprising a first region for performing an endothermic reaction, a second region for performing an exothermic reaction and the reactor assembly being arranged to transfer heat between the first and second regions, wherein the reactor assembly includes a diffusion bonded heat exchanger having two sets of channels formed therein with the first set of channels forming at least part of the first region, the second set of channels forming at least part of the second region and the diffusion bonded heat exchanger being arranged to transfer heat between the two sets of channels.
- a diffusion bonded heat exchanger is very compact and provides very good heat transfer between the first set of channels forming at least part of the first region and the second set of channels forming at least part of the second region.
- Experimental work has demonstrated that heat fluxes higher than 10 kW/m 2 can be achieved.
- the good heat transfer enables the reactions in each region to be performed more effectively and low thermal inertia provides faster start-up and better load following characteristics than conventional reactors.
- the use of a diffusion bonded heat exchanger produces a very compact and very effective reactor.
- the first region may for example be arranged to be supplied with steam and fuel gas to perform an endothermic steam reforming reaction.
- the second region may be arranged to be supplied with fuel to be combusted.
- the reactor When the reactor is used as a steam reformer its compact size and very high heat transfer rate make it particularly suitable for use to produce hydrogen for fuel cell systems for both stationary power plant and in fuel cell systems for mobile applications.
- the first region may be arranged to perform some other reaction such as an endothermic partial oxidation reaction.
- Table 1 below shows the energy density of the prior art steam reformers discussed above when used to supply hydrogen to a fuel cell which provides energy, compared to a steam reformer using the diffusion bonded reactor of the present invention.
- the diffusion bonded reactor of the present invention has an energy density which is orders of magnitude better than previous reactors and so a dramatic reduction in reformer volume and weight is achieved for production of the same amount of hydrogen/energy.
- At least some of either or both sets of channels may be provided with catalyst to assist the reaction to be performed in those channels.
- the catalyst is preferably coated onto the inside surface of the channels as a film.
- the catalyst may be provided as particles contained within the channels by for example a mesh at each end of the channels.
- Figure 1 diagrammatically shows a diffusion bonded heat exchanger forming a reactor
- Figure 2 diagrammatically shows another diffusion bonded heat exchanger forming a reactor with the channels in a different arrangement
- Figure 3 illustrates a steam reforming reaction and a combustion reaction performed within the reactor
- Figure 4 is a flow diagram of a reactor used as a steam reformer to supply hydrogen to a fuel cell.
- the diffusion bonded heat exchanger 10 illustrated in Figure 1 is a solid body 11 with three opposite pairs of sides 20, 30; 40, 50; 60, 70; with each opposite side being substantially parallel and identical to the other.
- Two opposite sides 20, 30 have a set of channels or passages 21 passing between them through the body of the heat exchanger 10 (only some of which are shown), for the passage of fluid therethrough.
- Two other opposite sides 40, 50 have a second set of channels or passages 41 passing between them through the heat exchange body 10 (only some of which are shown), in the example of Figure 1 in an orthogonal direction to the first set of channels 21 also for the passage of fluid therethrough.
- Each passage 21, 41 passes from one side 20, 40 to the opposite side 30, 50 without coming into fluid communication with channels passing in the orthogonal direction between two other opposite pairs of sides.
- the diffusion bonded heat exchanger 10 may be formed by any suitable method as is well known to the skilled man. Formation generally comprises the provision of a number of plates, some or all of which are provided with suitable channels. The plates are stacked with channels appropriately orientated. The stack is then subjected to appropriate heat and pressure for the plates to be diffusion bonded together to form a solid block with at least two sets of passages therethrough. To produce an equivalent amount of heat exchange between two sets of flow channels, a conventional heat exchanger formed of welded or brazed plates would have to be many times larger and heavier than its diffusion bonded equivalent.
- the diffusion bonded heat exchanger offers a very compact design with a surface density of up to 5000 m /m .
- the material used in the reactor depends on several factors such as long term strength (creep resistance), corrosion resistance, catalyst coating characteristics, fabrication limitations and cost. When used as a steam reformer, the reactor will need to handle gases in the temperature range 650°C - 850°C and pressure from 1 bar to about 8 bar.
- Many metals are suitable for this purpose such as relatively low cost conventional stainless steel, alloyed iron such as iron-chromium alloy which has established catalyst coating characteristics, Nl-based alloys with increased high temperature strength and oxide dispersion strength alloys. Ceramic materials such as alumina may also be used, especially when the reactor is used at high temperatures.
- a manifold may be positioned over each of the sides 20, 30, 40, 50 to supply fluid to or receive fluid from the channels 21, 41.
- a first manifold is arranged to supply steam and fuel, preferably fuel gas such as natural gas or methane to one side 20 containing the first set of channels 21.
- the fuel and steam is arranged to react in the channels 21 which act as the first reaction region and the products of the reaction pass through the channels 21 to the opposite side 30 of the heat exchanger 10 to be received by a second manifold (not shown).
- the channels 21 acting as the first reaction region are preferably provided with catalyst to increase the reaction rate as described later.
- a third manifold may be arranged to supply fluids to another side 40 of the heat exchanger containing entrances to the second set of channels 41.
- the fluids delivered by the third manifold are arranged to react within the second set of channels 41 acting as the second reaction region.
- the products of the reaction in the second region pass through the second set of channels 41 and are received by a fourth manifold positioned over the side 50 of the heat exchanger opposite to the side arranged to receive the third manifold.
- the second set of channels is preferably arranged to perform an exothermic reaction such as combustion of fuel, preferably fuel gas such as natural gas or methane. Catalyst may be provided within the second set of channels 41 as described later.
- the channels need not necessarily pass between opposite sides of the heat exchanger but could pass between any two parts of the heat exchanger as is convenient.
- the first 21 and second 41 sets of channels may pass through the body 1 1 of the heat exchanger 10 between different portions 22, 23; 42, 43 of the same side 20; 40 as diagrammatically shown in Figure 2 or between adjacent sides (not shown).
- the channels are arranged, it is preferable that the first 21 and second 41 sets of channels overlap each other or are interleaved for enhanced heat transfer between the endothermic and exothermic regions.
- the heat exchanger 10 may not be a parallelepiped but may be of any shape as is convenient.
- Catalyst is preferably deposited directly onto the heat exchange surface of either or both of the sets of channels 21, 41. Catalyst is preferably coated onto the inside surface of either or both of the sets of channels 21, 41 as a film. When catalyst is deposited on both sets of channels 21, 41 the catalysed regions can exchange heat directly with each other..
- the preferred method of coating the film is by using a sol-gel as is well known in the art (see for example 'Fundamental Principles of Sol-Gel Technology' by R W Jones published by the Institute of Materials 1989) and which may be applied to the inside surface of the desired channels by established methods such as by being blown through the channels by a stream of air.
- catalyst may be provided as small particles located within either or both sets of heat reformer channels 21, 41. The catalyst particles may be maintained within the appropriate channels by a mesh at each end.
- Figure 3 diagramatically shows the reactions performed in adjacent channels 21, 41 when the heat exchanger 10 of the reactor is used as a steam reformer.
- Channels 41 shown coated with a catalyst film 45 receive a stream of fuel, in this case methane which is combusted with air in the presence of the catalyst 45 and produced heat passes through the body 11 of the heat exchanger 10 to channels 21 in which a steam reforming reaction is performed.
- Channel 21 receives a fuel stream, in this case methane and water to produce hydrogen in the presence of catalyst film 25.
- the heat received from surrounding channels 41 promotes the steam reforming reaction increasing hydrogen yield.
- Platinum (Pt) and palladium (Pd) are among the most active catalysts for the catalytic combustion of a range of fuels including natural gas. Palladium has been found to have a higher activity for methane combustion. Other noble metals may be used. Rhodium is used, for example in automotive exhaust catalysts while iridium and ruthenium added to catalyst formulations have been found to reduce the tendency of the catalyst to sinter and deactivate. Noble metal combustion catalysts exhibit high activity. Platinum and palladium based catalysts may operate at temperatures up to 1300°C. The use of the reactor of the present invention as a compact reformer thus does not pose any temperature restrictions on the use of Pd or Pt catalysts, and these are the preferred option.
- the catalyst support is also important for the reformer.
- Traditional pelleted catalysts use supports of alumina or silica to maximise the surface area and give good dispersion of the active metal.
- the most widely used support is gamma-alumina.
- stabilisers may be added to the support to minimise the sintering of the support, brought about by a phase change from gamma to alpha alumina.
- Stabilisers such as CeO 2 or CsO 2 may be added to the support, to raise the temperature at which sintering commences. In the present case un-doped gamma alumina has been used.
- a thin film Pd/alumina combustion catalyst was prepared as follows.
- a palladium nitrate/alumina sol was made up by dissolving palladium nitrate hydrate (0.225g)
- Nickel has become the most widely used catalyst metal in industry for the steam reforming of hydrocarbons.
- Other metals such as Co, Ru, Rh, Pd, Pt, Ir may be used but are generally avoided on cost grounds, despite the fact that their intrinsic catalytic activity may be higher, and that they may be less active in promoting carbon forming reactions.
- Ni catalysts and Ru catalysts that were prepared and applied using a sol-gel method. Ru was used because of its good resistance to sulphur and carbon deposition.
- the principal effect in the reactor 10 is that of reaction rates which is in itself influenced by the residence time.
- the residence time within each channel 21, 41 of the heat exchanger 10 is influenced primarily by its diameter.
- Experimentation examined the effect of changing the channel dimensions on the temperature profile. A selection of results is presented in Table 2.
- the cross-sectional area of the combustion channels 41 is preferably larger than that of the reforming channels 21.
- the cross-sectional area of the combustion channels 41 may be twice, five times or even ten times that of the reforming channels 21.
- the cross-sectional area of the combustion channels 41 may be half, a fifth or even a tenth of that of the reforming channels 21.
- the diameter of the combustion channel 41 is preferably between 10 and 30 mm and the reforming channel diameter is preferably between 1 and 3 mm.
- the channels 21, 41 may have an aspect ratio within the range of substantially 1 to 10 and may have a substantially circular cross-section.
- the influence of residence time on temperature leads to a method of controlling the temperature of the reactor. That is by controlling the flow of fuel and oxidant to the combustion side, for example by using suitable valves, it is possible to control the heat released to the reformer and thereby control the conversion of reforming.
- the performance of the reformer can thus be controlled by applying flow controls to the combustion inlet.
- the Tables 3 and 4 below show the operating conditions for the reactor of the present invention when used as a steam reformer to provide sufficient hydrogen for a 200 kW fuel cell system. For a typical system efficiency this requires a natural gas feed rate of 1.8 kmol/h on the reforming side and 0.4 kmol/h on the combustion side. Based on these figures, the weight
- FIG. 4 An example of the reactor used as a reformer to supply hydrogen to a fuel cell is shown in Figure 4. Reforming of fuel gas external to a fuel cell stack is a fundamental requirement for all fuel cell systems employing low temperature stacks such as the Solid Polymer Fuel Cell
- SPFC Proton Exchange Membrane
- AFC Alkaline Fuel Cell
- PAFC Phosphoric Acid Fuel Cell
- FIG. 4 An example of a process design for an SPFC fuel cell system employing a reformer of the present invention is shown in Figure 4.
- the reformer 100 is arranged to operate at 750°C and in the combustion section 41 air supplied through inlet 101 is set at 100% excess (i.e. 2 x stoichometric).
- the reformer 100 is assumed to be a co-current flow design and air is pre-heated to above the combustion light-off temperature by exchanging heat from a heat exchanger 103 through which gases produced by combustion in the reformer 100 pass via outlet 102.
- Fuel gas in this case natural gas, is supplied to reformer 100 via inlet 104 to be combusted with air from inlet 101.
- Steam is raised from a water supply inlet 105 which passes through and takes heat from gases leaving the reforming section 21 of the reformer 100 via a heat exchanger 106.
- the water is combined with fuel gas, in this case natural gas from inlet 107 and which optionally passes through a desulphurisation vessel 108.
- the fuel gas/steam mixture is supplied to the reforming channels 21 of the reformer 100 by conduit 109.
- Hydrogen produced in the reformer 100 is supplied via conduit 110 to a fuel cell (not shown).
- the preheat possible in the scheme depends on how the heat integration is performed. Studies have shown that preheat temperatures in excess of 700°C are possible with the heat available from elsewhere in the system such as using the heat from the combustion exhaust gases from the reformer 100 in outlet 102 for heat exchange with the input air.
- a combustor 111 is used to further heat the combustion exhaust gases in outlet 102.
- each set of channels 21, 41 in the diffusion bonded heat exchanger could comprise one or more channels. These channels could pass back and forth within the heat exchange body 11 to increase the heat exchange effect.
- catalyst may be provided as a film on the inside surface of one set of channels and provided as particles in the other set of channels.
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Abstract
Description
Claims
Priority Applications (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
CA002380823A CA2380823A1 (en) | 1999-08-07 | 2000-07-31 | Compact reactor |
EP00949713A EP1208061A1 (en) | 1999-08-07 | 2000-07-31 | Compact reactor |
JP2001515248A JP2003506306A (en) | 1999-08-07 | 2000-07-31 | Compact reactor |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
GBGB9918586.0A GB9918586D0 (en) | 1999-08-07 | 1999-08-07 | Compact reactor |
GB9918586.0 | 1999-08-07 |
Publications (1)
Publication Number | Publication Date |
---|---|
WO2001010773A1 true WO2001010773A1 (en) | 2001-02-15 |
Family
ID=10858722
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/GB2000/002887 WO2001010773A1 (en) | 1999-08-07 | 2000-07-31 | Compact reactor |
Country Status (5)
Country | Link |
---|---|
EP (1) | EP1208061A1 (en) |
JP (1) | JP2003506306A (en) |
CA (1) | CA2380823A1 (en) |
GB (2) | GB9918586D0 (en) |
WO (1) | WO2001010773A1 (en) |
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US11661553B2 (en) | 2015-06-12 | 2023-05-30 | Velocys, Inc. | Synthesis gas conversion process |
US11959709B2 (en) | 2018-06-27 | 2024-04-16 | Welcon Inc. | Heat transport device and method for manufacturing same |
US12061053B2 (en) | 2018-06-27 | 2024-08-13 | Welcon Inc. | Heat transport device and method for manufacturing same |
Also Published As
Publication number | Publication date |
---|---|
CA2380823A1 (en) | 2001-02-15 |
GB2353801B (en) | 2003-04-30 |
GB2353801A (en) | 2001-03-07 |
JP2003506306A (en) | 2003-02-18 |
EP1208061A1 (en) | 2002-05-29 |
GB9918586D0 (en) | 1999-10-06 |
GB0018671D0 (en) | 2000-09-13 |
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