CN109126658A - A kind of micro passage reaction and its method of dehydrogenating of the dehydrogenation reaction suitable for liquid hydrogen source material - Google Patents
A kind of micro passage reaction and its method of dehydrogenating of the dehydrogenation reaction suitable for liquid hydrogen source material Download PDFInfo
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- CN109126658A CN109126658A CN201811089453.0A CN201811089453A CN109126658A CN 109126658 A CN109126658 A CN 109126658A CN 201811089453 A CN201811089453 A CN 201811089453A CN 109126658 A CN109126658 A CN 109126658A
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- passage reaction
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- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 75
- 239000001257 hydrogen Substances 0.000 title claims abstract description 75
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 70
- 238000006243 chemical reaction Methods 0.000 title claims abstract description 55
- 239000000463 material Substances 0.000 title claims abstract description 37
- 239000007788 liquid Substances 0.000 title claims abstract description 36
- 238000006356 dehydrogenation reaction Methods 0.000 title claims abstract description 25
- 238000000034 method Methods 0.000 title claims abstract description 14
- 239000000758 substrate Substances 0.000 claims abstract description 68
- 238000003860 storage Methods 0.000 claims abstract description 22
- 239000003054 catalyst Substances 0.000 claims abstract description 17
- 238000000926 separation method Methods 0.000 claims abstract description 12
- 239000012774 insulation material Substances 0.000 claims abstract description 6
- 238000005485 electric heating Methods 0.000 claims abstract description 5
- 239000002184 metal Substances 0.000 claims description 23
- 229910052751 metal Inorganic materials 0.000 claims description 23
- 238000001354 calcination Methods 0.000 claims description 18
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 claims description 15
- KYQCOXFCLRTKLS-UHFFFAOYSA-N Pyrazine Chemical compound C1=CN=CC=N1 KYQCOXFCLRTKLS-UHFFFAOYSA-N 0.000 claims description 12
- 239000011248 coating agent Substances 0.000 claims description 11
- 238000000576 coating method Methods 0.000 claims description 11
- 238000006722 reduction reaction Methods 0.000 claims description 10
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims description 9
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 claims description 9
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 claims description 9
- QGJOPFRUJISHPQ-UHFFFAOYSA-N Carbon disulfide Chemical compound S=C=S QGJOPFRUJISHPQ-UHFFFAOYSA-N 0.000 claims description 9
- YMWUJEATGCHHMB-UHFFFAOYSA-N Dichloromethane Chemical compound ClCCl YMWUJEATGCHHMB-UHFFFAOYSA-N 0.000 claims description 9
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 claims description 9
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 9
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 9
- -1 arene compound Chemical class 0.000 claims description 9
- RTZKZFJDLAIYFH-UHFFFAOYSA-N ether Substances CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 9
- 125000000623 heterocyclic group Chemical group 0.000 claims description 9
- 150000003839 salts Chemical class 0.000 claims description 9
- 239000012298 atmosphere Substances 0.000 claims description 8
- 150000001875 compounds Chemical class 0.000 claims description 8
- 239000002904 solvent Substances 0.000 claims description 7
- 229910003158 γ-Al2O3 Inorganic materials 0.000 claims description 7
- PAYRUJLWNCNPSJ-UHFFFAOYSA-N Aniline Chemical compound NC1=CC=CC=C1 PAYRUJLWNCNPSJ-UHFFFAOYSA-N 0.000 claims description 6
- UJOBWOGCFQCDNV-UHFFFAOYSA-N Carbazole Natural products C1=CC=C2C3=CC=CC=C3NC2=C1 UJOBWOGCFQCDNV-UHFFFAOYSA-N 0.000 claims description 6
- HEDRZPFGACZZDS-UHFFFAOYSA-N Chloroform Chemical compound ClC(Cl)Cl HEDRZPFGACZZDS-UHFFFAOYSA-N 0.000 claims description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- YNQLUTRBYVCPMQ-UHFFFAOYSA-N Ethylbenzene Chemical compound CCC1=CC=CC=C1 YNQLUTRBYVCPMQ-UHFFFAOYSA-N 0.000 claims description 6
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 6
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 claims description 6
- UFWIBTONFRDIAS-UHFFFAOYSA-N Naphthalene Chemical compound C1=CC=CC2=CC=CC=C21 UFWIBTONFRDIAS-UHFFFAOYSA-N 0.000 claims description 6
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical group CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 claims description 6
- OFBQJSOFQDEBGM-UHFFFAOYSA-N Pentane Chemical compound CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 claims description 6
- PCNDJXKNXGMECE-UHFFFAOYSA-N Phenazine Natural products C1=CC=CC2=NC3=CC=CC=C3N=C21 PCNDJXKNXGMECE-UHFFFAOYSA-N 0.000 claims description 6
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 claims description 6
- JUJWROOIHBZHMG-UHFFFAOYSA-N Pyridine Chemical compound C1=CC=NC=C1 JUJWROOIHBZHMG-UHFFFAOYSA-N 0.000 claims description 6
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 claims description 6
- MWPLVEDNUUSJAV-UHFFFAOYSA-N anthracene Chemical compound C1=CC=CC2=CC3=CC=CC=C3C=C21 MWPLVEDNUUSJAV-UHFFFAOYSA-N 0.000 claims description 6
- IOJUPLGTWVMSFF-UHFFFAOYSA-N benzothiazole Chemical compound C1=CC=C2SC=NC2=C1 IOJUPLGTWVMSFF-UHFFFAOYSA-N 0.000 claims description 6
- RWGFKTVRMDUZSP-UHFFFAOYSA-N cumene Chemical compound CC(C)C1=CC=CC=C1 RWGFKTVRMDUZSP-UHFFFAOYSA-N 0.000 claims description 6
- IVSZLXZYQVIEFR-UHFFFAOYSA-N m-xylene Chemical group CC1=CC=CC(C)=C1 IVSZLXZYQVIEFR-UHFFFAOYSA-N 0.000 claims description 6
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 claims description 6
- YNPNZTXNASCQKK-UHFFFAOYSA-N phenanthrene Chemical compound C1=CC=C2C3=CC=CC=C3C=CC2=C1 YNPNZTXNASCQKK-UHFFFAOYSA-N 0.000 claims description 6
- ODLMAHJVESYWTB-UHFFFAOYSA-N propylbenzene Chemical compound CCCC1=CC=CC=C1 ODLMAHJVESYWTB-UHFFFAOYSA-N 0.000 claims description 6
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 claims description 5
- 230000000694 effects Effects 0.000 claims description 5
- 239000000126 substance Substances 0.000 claims description 5
- 230000005484 gravity Effects 0.000 claims description 4
- 150000002431 hydrogen Chemical class 0.000 claims description 4
- 239000003208 petroleum Substances 0.000 claims description 4
- SCYULBFZEHDVBN-UHFFFAOYSA-N 1,1-Dichloroethane Chemical class CC(Cl)Cl SCYULBFZEHDVBN-UHFFFAOYSA-N 0.000 claims description 3
- DURPTKYDGMDSBL-UHFFFAOYSA-N 1-butoxybutane Chemical compound CCCCOCCCC DURPTKYDGMDSBL-UHFFFAOYSA-N 0.000 claims description 3
- QRRKZFCXXBFHSV-UHFFFAOYSA-N 1-ethylindole Chemical compound C1=CC=C2N(CC)C=CC2=C1 QRRKZFCXXBFHSV-UHFFFAOYSA-N 0.000 claims description 3
- BLRHMMGNCXNXJL-UHFFFAOYSA-N 1-methylindole Chemical compound C1=CC=C2N(C)C=CC2=C1 BLRHMMGNCXNXJL-UHFFFAOYSA-N 0.000 claims description 3
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 claims description 3
- PLAZXGNBGZYJSA-UHFFFAOYSA-N 9-ethylcarbazole Chemical compound C1=CC=C2N(CC)C3=CC=CC=C3C2=C1 PLAZXGNBGZYJSA-UHFFFAOYSA-N 0.000 claims description 3
- SDFLTYHTFPTIGX-UHFFFAOYSA-N 9-methylcarbazole Chemical compound C1=CC=C2N(C)C3=CC=CC=C3C2=C1 SDFLTYHTFPTIGX-UHFFFAOYSA-N 0.000 claims description 3
- LSZJZNNASZFXKN-UHFFFAOYSA-N 9-propan-2-ylcarbazole Chemical compound C1=CC=C2N(C(C)C)C3=CC=CC=C3C2=C1 LSZJZNNASZFXKN-UHFFFAOYSA-N 0.000 claims description 3
- QAWLNVOLYNXWPL-UHFFFAOYSA-N 9-propylcarbazole Chemical compound C1=CC=C2N(CCC)C3=CC=CC=C3C2=C1 QAWLNVOLYNXWPL-UHFFFAOYSA-N 0.000 claims description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 claims description 3
- 229910002706 AlOOH Inorganic materials 0.000 claims description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 claims description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 3
- ZAFNJMIOTHYJRJ-UHFFFAOYSA-N Diisopropyl ether Chemical compound CC(C)OC(C)C ZAFNJMIOTHYJRJ-UHFFFAOYSA-N 0.000 claims description 3
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical group COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 claims description 3
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 3
- FZWLAAWBMGSTSO-UHFFFAOYSA-N Thiazole Chemical compound C1=CSC=N1 FZWLAAWBMGSTSO-UHFFFAOYSA-N 0.000 claims description 3
- 229950005499 carbon tetrachloride Drugs 0.000 claims description 3
- FMGSKLZLMKYGDP-USOAJAOKSA-N dehydroepiandrosterone Chemical class C1[C@@H](O)CC[C@]2(C)[C@H]3CC[C@](C)(C(CC4)=O)[C@@H]4[C@@H]3CC=C21 FMGSKLZLMKYGDP-USOAJAOKSA-N 0.000 claims description 3
- 235000019441 ethanol Nutrition 0.000 claims description 3
- 235000019253 formic acid Nutrition 0.000 claims description 3
- WBJINCZRORDGAQ-UHFFFAOYSA-N formic acid ethyl ester Natural products CCOC=O WBJINCZRORDGAQ-UHFFFAOYSA-N 0.000 claims description 3
- 150000002240 furans Chemical class 0.000 claims description 3
- 125000004836 hexamethylene group Chemical group [H]C([H])([*:2])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[*:1] 0.000 claims description 3
- 150000002475 indoles Chemical class 0.000 claims description 3
- 229910052742 iron Inorganic materials 0.000 claims description 3
- 229910044991 metal oxide Inorganic materials 0.000 claims description 3
- 150000004706 metal oxides Chemical class 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- TVMXDCGIABBOFY-UHFFFAOYSA-N octane Chemical compound CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 claims description 3
- 150000003891 oxalate salts Chemical class 0.000 claims description 3
- 229910052763 palladium Inorganic materials 0.000 claims description 3
- 229910052697 platinum Inorganic materials 0.000 claims description 3
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 claims description 3
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 claims description 3
- 150000003233 pyrroles Chemical class 0.000 claims description 3
- 229910052703 rhodium Inorganic materials 0.000 claims description 3
- 229910052707 ruthenium Inorganic materials 0.000 claims description 3
- VZGDMQKNWNREIO-UHFFFAOYSA-N tetrachloromethane Chemical compound ClC(Cl)(Cl)Cl VZGDMQKNWNREIO-UHFFFAOYSA-N 0.000 claims description 3
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 claims description 2
- 150000001335 aliphatic alkanes Chemical class 0.000 claims description 2
- 125000000609 carbazolyl group Chemical group C1(=CC=CC=2C3=CC=CC=C3NC12)* 0.000 claims description 2
- 239000003365 glass fiber Substances 0.000 claims description 2
- 239000011490 mineral wool Substances 0.000 claims description 2
- 229920002635 polyurethane Polymers 0.000 claims description 2
- 239000004814 polyurethane Substances 0.000 claims description 2
- 235000003642 hunger Nutrition 0.000 claims 1
- 229910001960 metal nitrate Inorganic materials 0.000 claims 1
- 239000000203 mixture Substances 0.000 claims 1
- 238000012546 transfer Methods 0.000 abstract description 6
- 239000007789 gas Substances 0.000 description 6
- 238000010586 diagram Methods 0.000 description 5
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 229910002651 NO3 Inorganic materials 0.000 description 2
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 2
- URLKBWYHVLBVBO-UHFFFAOYSA-N Para-Xylene Chemical group CC1=CC=C(C)C=C1 URLKBWYHVLBVBO-UHFFFAOYSA-N 0.000 description 2
- 239000003153 chemical reaction reagent Substances 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 238000005253 cladding Methods 0.000 description 2
- 239000000446 fuel Substances 0.000 description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 2
- 229910052737 gold Inorganic materials 0.000 description 2
- 239000010931 gold Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 2
- 239000003345 natural gas Substances 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 230000036632 reaction speed Effects 0.000 description 2
- 239000011877 solvent mixture Substances 0.000 description 2
- SQFONLULGFXJAA-UHFFFAOYSA-N 9-butylcarbazole Chemical compound C1=CC=C2N(CCCC)C3=CC=CC=C3C2=C1 SQFONLULGFXJAA-UHFFFAOYSA-N 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 150000003851 azoles Chemical class 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 238000010924 continuous production Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 1
- 230000002779 inactivation Effects 0.000 description 1
- 150000004702 methyl esters Chemical class 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 238000004321 preservation Methods 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
Classifications
-
- 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
- B01J19/0093—Microreactors, e.g. miniaturised or microfabricated reactors
-
- 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
- C01B3/0005—Reversible uptake of hydrogen by an appropriate medium, i.e. based on physical or chemical sorption phenomena or on reversible chemical reactions, e.g. for hydrogen storage purposes ; Reversible gettering of hydrogen; Reversible uptake of hydrogen by electrodes
- C01B3/001—Reversible uptake of hydrogen by an appropriate medium, i.e. based on physical or chemical sorption phenomena or on reversible chemical reactions, e.g. for hydrogen storage purposes ; Reversible gettering of hydrogen; Reversible uptake of hydrogen by electrodes characterised by the uptaking medium; Treatment thereof
- C01B3/0015—Organic compounds; Solutions thereof
-
- 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
- C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
-
- 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
- Y02E60/32—Hydrogen storage
-
- 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
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- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- General Health & Medical Sciences (AREA)
- Engineering & Computer Science (AREA)
- Combustion & Propulsion (AREA)
- Inorganic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Hydrogen, Water And Hydrids (AREA)
Abstract
The invention belongs to hydrogen storage catalyst technical fields, disclose the micro passage reaction and its method of dehydrogenating of a kind of dehydrogenation reaction suitable for liquid hydrogen source material.The micro passage reaction is cylindrical, including outer wall, inlet tube, substrate, gas-liquid separation chamber, outlet tube and escape pipe；Several inlet openings are offered on inlet tube, it is connect upwardly through inlet opening with substrate in the Vertical Square of inlet tube, catalyst coat is coated on substrate, substrate is made of several deflectors, and electric heating wire is provided in substrate, flow-disturbing point is provided on substrate, microchannel is formed between substrate, gas-liquid separation chamber is the region between substrate and outer wall, and escape pipe is located at the top of micro passage reaction, outlet tube is located at the bottom of micro passage reaction, and outer wall coats thermal insulation material.Micro passage reaction of the invention has great specific surface area, is provided in microchannel and upsets the protrusion of flowing, has fabulous heat transfer and mass transfer ability, the moment that material may be implemented uniformly mixes and efficient heat transfer.
Description
Technical field
The invention belongs to hydrogen storage technology fields, more particularly, to a kind of dehydrogenation reaction suitable for liquid hydrogen source material
Micro passage reaction and its method of dehydrogenating.
Background technique
The fossil energies such as coal, petroleum, natural gas are the energy consumption main bodys of today's society, with constantly mentioning for total quantity consumed
Height is faced with reserves reduction, and exploitation difficulty increases, the predicament that production marginal cost rises.Research is thought, before the year two thousand twenty, entirely
Ballstone oil yield will reach vertex, and the vertex of gas production will also reach soon, following supply falls short of demand the gesture
It must lead to skyrocketing for oil and natural gas price in world wide.
Hydrogen Energy is generally acknowledged clean energy resource, is known as 21 century secondary energy sources most with prospects, it helps to solve
Energy crisis, global warming and environmental pollution, development and utilization have obtained worldwide highest attention.Hydrogen has cleaning
Pollution-free, storage and transportation is convenient, utilization rate is high, the characteristics of chemical energy being converted directly into electric energy by fuel cell, meanwhile, hydrogen
It is from a wealth of sources, produce approach multiplicity.
High-pressure hydrogen storing bottle used at present, solid metal hydrogen storage, there is high pressure hydrogens easily to reveal for porous material hydrogen storage, expensive
Metal hydrogen storage cost is excessively high, and porous material hydrogen storage is recycled the problems such as number is limited and the use of hydrogen energy source is restricted.It is existing
Modern more reliable hydrogen storage and discharge mode has aqueous chemical hydrogen storage mode, and hydrogen is stored in hydrogen storage carrier in a manner of chemical state
Interior, in the presence of suitable pressure and temp catalyst, hydrogen in hydrogen storage carrier by releasing.Conventional tank reactor there is
Response area is smaller, and reaction speed is slow, and catalyst in whipping process the problems such as easily broken inactivation, develop a kind of efficiently anti-by urgent need
Device is answered to cope with vehicle fuel battery hydrogen demand in future.
Summary of the invention
In order to solve above-mentioned the shortcomings of the prior art and disadvantage, it is an object of that present invention to provide one kind to be suitable for liquid
The micro passage reaction of the dehydrogenation reaction of hydrogen source material effectively improves reactivity of the catalyst in micro passage reaction, anti-
Poisoning capability, carbon accumulation resisting ability and service life, and have many advantages, such as that apparatus module, continuous production, catalyst are easy to regenerate.
Another object of the present invention is to provide the method for dehydrogenating of above-mentioned micro passage reaction.
The purpose of the present invention is realized by following technical proposals:
A kind of micro passage reaction of the dehydrogenation reaction suitable for liquid hydrogen source material, the micro passage reaction cylinder
Shape, including outer wall, inlet tube, substrate, gas-liquid separation chamber, outlet tube and escape pipe；Several feed liquors are offered on the inlet tube
Hole connect with the substrate upwardly through the inlet opening in the Vertical Square of the inlet tube, is coated with catalysis on the substrate
Agent coating, the substrate are made of several deflectors, and electric heating wire is provided in the substrate, is provided with flow-disturbing on the substrate
Point forms microchannel between the substrate, and the gas-liquid separation chamber is the region between the substrate and the outer wall, it is described go out
Tracheae is located at the top of the micro passage reaction, and the outlet tube is located at the bottom of micro passage reaction, the outer wall cladding
Thermal insulation material.
Further, the number of the substrate is 2~1000, and the shape of the substrate is straight panel, wave-shape board or folded plate
One or more of, the number of the deflector is 2~32, and the diameter of the substrate is the micro passage reaction diameter
0.1~0.9 times.
Preferably, the thermal insulation material is one or more of glass fibre, polyurethane, rock wool, pearlife or aeroge.
Further, the flow-disturbing point is circular protrusions or square protrusion.
Preferably, the microchannel with a thickness of 50~2000 microns；
Preferably, the catalyst coat is metal layer, and the metal layer is that AlOOH sol layer is first coated on substrate,
γ-Al is generated by calcining I2O3Coating, then again in γ-Al2O3Metal salt is coated on coating as presoma, in sky
Under gas or inert atmosphere, metal oxide is obtained by calcining II, in a hydrogen atmosphere, reduction reaction is carried out and is made.
It is further preferable that the metal layer is one or more of Pt, Rh, Ru, Pd, Ni, Co, Mg, Ca or Fe, the gold
Belong to nitrate, acetate, oxalates, carbonate, bicarbonate, sulfate or the chloride that salt is above-mentioned metal, the inertia
Atmosphere is N2, Ar or He；The temperature of the calcining I is 300~600 DEG C, and the temperature of the calcining II is 200~550 DEG C, institute
The temperature for stating reduction reaction is 200~500 DEG C；The calcining I and calcining II, the time of reduction reaction is 3~8h, the gold
Belong to layer, γ-Al2O3Coating, metal salt thickness be 10~100 microns.
The method of dehydrogenating of the micro passage reaction of the dehydrogenation reaction suitable for liquid hydrogen source material, specific steps
It is as follows:
S1. the preheated device of hydrogen source material is preheated to 80-300 DEG C, and the inlet tube through bottom inputs micro passage reaction, hydrogen source
Material is uniformly distributed by the inlet opening on inlet tube into the microchannel being made of the gap between substrate；
S2. on the catalyst coat in microchannel, hydrogen source material is broken down into hydrogen storage carrier and hydrogen, and product leads to from micro-
Road outlet enters gas-liquid separation chamber, and under the effect of gravity, hydrogen storage carrier, which flows downward, is discharged micro passage reaction, hydrogen through outlet tube
Gas, which rises, is discharged micro passage reaction by escape pipe, completes Dehydroepiandrosterone derivative.
Preferably, hydrogen storage carrier described in step S2 is unsaturated arene compound and/or heterocycle unsaturated compound
One of or a variety of with solvent mixture, the unsaturation arene compound and/or heterocycle unsaturated compound: solvent
Mass ratio be (0.03~0.97): 1.
Preferably, the unsaturated arene compound be benzene, toluene, ethylbenzene, propyl benzene, isopropylbenzene, ortho-xylene, to two
Toluene, meta-xylene, styrene, naphthalene, anthracene, phenanthrene, phenol, aniline or its above-mentioned substance derivative；The heterocycle unsaturation
Conjunction object is carbazole, indoles, N- methyl carbazole, N- ethyl carbazole, N- n-propyl carbazole, N- isopropylcarbazole, N- normal-butyl click
Azoles, N- methyl indol, N- ethylindole, pyrazine, furans, pyrroles, thiazole, pyridine, penta pyrazine of ring, benzothiazole and its derivative
Object；The solvent be methanol, ethyl alcohol, isopropanol, ethylene glycol, normal propyl alcohol, n-butanol, ether, methyl ether, acetonitrile, formic acid, acetic acid,
Ethyl acetate, methyl acetate, Ethyl formate, n-butyl ether, isopropyl ether, methylene chloride, chloroform, tetrachloromethane, dichloroethanes, just oneself
One or more of alkane, hexamethylene, pentane, normal octane, carbon disulfide or petroleum ether.
Compared with prior art, the invention has the following advantages:
1. micro passage reaction of the invention, which will react scale, is contracted to micron order, and is catalyzed using the nanoscale of high activity
Agent coating greatly improves the efficiency of reaction, reduces reactor size, reduces equipment investment cost.
2. micro passage reaction of the invention has great specific surface area, the hundred times of reachable stirred tank specific surface area are very
To thousands of times.The protrusion for upsetting and flowing is provided in microchannel may be implemented object to reach fabulous heat transfer and mass transfer ability
The moment of material uniformly mixes and efficient heat transfer.
3. deflector is arranged in micro passage reaction of the invention, liquid can be allowed more uniformly to be distributed, improve catalyst coat
Utilization rate, improve reaction speed.
Detailed description of the invention
Fig. 1 is micro passage reaction front cross-sectional view of the present invention.
Fig. 2 is the schematic top plan view of substrate of the present invention.
Fig. 3 is that flow-disturbing point uses circular protrusions schematic diagram on substrate of the present invention.
Fig. 4 is that flow-disturbing point uses square bump diagrams on substrate of the present invention.
Fig. 5 is that substrate of the present invention uses wave-shape board schematic diagram.
Fig. 6 is that substrate of the present invention uses straight panel schematic diagram.
Fig. 7 is that substrate of the present invention uses folded plate schematic diagram.
Specific embodiment
The contents of the present invention are further illustrated combined with specific embodiments below, but should not be construed as limiting the invention.
Unless otherwise specified, the conventional means that technological means used in embodiment is well known to those skilled in the art.Except especially saying
Bright, reagent that the present invention uses, method and apparatus is the art conventional reagents, method and apparatus.
Embodiment 1
The present invention provides a kind of micro passage reaction of dehydrogenation reaction suitable for liquid hydrogen source material, Fig. 1 is micro- logical
Road reactor front cross-sectional view.Micro passage reaction includes outer wall, inlet tube 1, inlet opening 2, substrate 3, gas-liquid separation chamber 4, out
Tracheae 5 and outlet tube 6.Wherein, micro passage reaction is cylinder, and inlet tube 1 is located at bottom the center point, passes straight through to instead from bottom
Answer at the top of device, offer several inlet openings 2 on the inlet tube 1, the inlet tube 1 Vertical Square upwardly through the feed liquor
Hole 2 is connect with the substrate 3.Fig. 2 is the schematic top plan view of substrate.Catalyst coat, the substrate are coated on the substrate 3
3, which are divided into multiple sectors by several deflectors 9, forms, and electric heating wire is provided in the substrate 3, if being provided on the substrate 3
Flow point 8 is interfered, forms microchannel between the substrate 3, the gas-liquid separation chamber 4 is the region between substrate 3 and outer wall, described
Escape pipe 5 is located at the top of the micro passage reaction, and the outlet tube 6 is located at the bottom of micro passage reaction, the outer wall
Coat insulating layer.
The shape of substrate described in the present embodiment is straight panel, as shown in Figure 6.
Flow-disturbing point uses circular protrusions in the present embodiment, as shown in Figure 3.
Specifically, the number of the substrate is 2~1000, and the number of the deflector is 2~32.
Specifically, the diameter of the substrate is 0.1~0.9 times of the micro passage reaction diameter.
Specifically, the microchannel with a thickness of 50~2000 microns.
Specifically, the insulating layer with a thickness of 100~1000mm.
Specifically, the catalyst coat is metal layer, and the metal layer is that AlOOH sol layer is first coated on substrate,
γ-Al is generated by calcining I2O3Coating, then again in γ-Al2O3Metal salt is coated on coating as presoma, in sky
Under gas or inert atmosphere, metal oxide is obtained by calcining II, reduction reaction is carried out in a hydrogen atmosphere and is made.
Specifically, the metal layer is one or more of Pt, Rh, Ru, Pd, Ni, Co, Mg, Ca or Fe, the metal salt
For the nitrate of above-mentioned metal, acetate, oxalates, carbonate, bicarbonate, sulfate or chloride, the temperature of the calcining I
Degree is 300~600 DEG C, and the temperature of the calcining II is 200~550 DEG C, and the temperature of the reduction reaction is 200~500 DEG C；Institute
Calcining I and calcining II are stated, the time of reduction reaction is 3~8h, the metal layer, γ-Al2O3The thickness of coating, metal salt
It is 10~100 microns.
The method of dehydrogenating of the micro passage reaction of the above-mentioned dehydrogenation reaction suitable for liquid hydrogen source material, specific steps are such as
Under:
S1. the preheated device of hydrogen source material is preheated to 80-300 DEG C, and the inlet tube through bottom inputs micro passage reaction, hydrogen source
Material is uniformly distributed by the inlet opening on inlet tube into the microchannel being made of the gap between substrate；
S2. on the catalyst coat in microchannel, hydrogen source material is broken down into hydrogen storage carrier and hydrogen, and product leads to from micro-
Road outlet enters gas-liquid separation chamber, and under the effect of gravity, hydrogen storage carrier, which flows downward, is discharged micro passage reaction, hydrogen through outlet tube
Gas, which rises, is discharged micro passage reaction by escape pipe, completes Dehydroepiandrosterone derivative.
Specifically, hydrogen storage carrier described in step S2 is unsaturated arene compound and/or heterocycle unsaturated compound
One of or a variety of with solvent mixture, the unsaturation arene compound and/or heterocycle unsaturated compound: solvent
Mass ratio=(0.03~0.97): 1.
Specifically, the unsaturated arene compound can for benzene, toluene, ethylbenzene, propyl benzene, isopropylbenzene, ortho-xylene,
Paraxylene, meta-xylene, styrene, naphthalene, anthracene, phenanthrene, phenol, aniline or derivatives thereof；The heterocycle unsaturated compound is
Carbazole, indoles, N- methyl carbazole, N- ethyl carbazole, N- n-propyl carbazole, N- isopropylcarbazole, N- normal-butyl carbazole, N- methyl
Indoles, N- ethylindole, pyrazine, furans, pyrroles, thiazole, pyridine, penta pyrazine of ring, benzothiazole and its derivative；The solvent
For methanol, ethyl alcohol, isopropanol, ethylene glycol, normal propyl alcohol, n-butanol, ether, methyl ether, acetonitrile, formic acid, acetic acid, ethyl acetate, second
Sour methyl esters, Ethyl formate, n-butyl ether, isopropyl ether, methylene chloride, chloroform, tetrachloromethane, dichloroethanes, n-hexane, hexamethylene,
One or more of pentane, normal octane, carbon disulfide or petroleum ether.
Embodiment 2
The present embodiment provides a kind of micro passage reactions of dehydrogenation reaction suitable for liquid hydrogen source material, with embodiment 1
Difference be, the flow-disturbing point using square protrusion, as shown in figure 4, the shape of the substrate be wave-shape board, as shown in Figure 5.
Embodiment 3
The present embodiment provides a kind of micro passage reactions of dehydrogenation reaction suitable for liquid hydrogen source material, with embodiment 1
Difference be, the flow-disturbing point using square protrusion, as shown in figure 4, the shape of the substrate be folded plate, as shown in Figure 7.
Embodiment 4
The present embodiment provides a kind of micro passage reaction of dehydrogenation reaction suitable for liquid hydrogen source material, microchannel plate is answered
Device is cylinder, and inlet tube 1 is located at bottom the center point, passes straight through to reactor head from bottom, be provided with inlet opening on inlet tube 1
2, inlet tube 1 is connected with substrate 3 in the horizontal direction, and the flow-disturbing point in the present embodiment on substrate is using square protrusion, such as Fig. 4 institute
Show.The substrate uses wave-shape board, folded plate and straight panel.It is coated with catalyst coat on substrate 3, is provided with electric heating in substrate 3
Thread, it is provided with deflector 9 on substrate 3, forms microchannel between substrate 3 and substrate 3, the diameter of substrate 3 is less than the straight of reactor
Diameter, the diameter of the substrate are 0.1~0.9 times of the micro passage reaction diameter.Region between substrate 3 and outer wall is gas
Liquid disengagement chamber 4, escape pipe 5 are located at the top of reactor, and outlet tube 6 is located at the bottom of reactor, outside cladding thermal insulation material pair
Entire reactor heat preservation.
When dehydrogenation works, hydrogen source material is preheated to 80~300 DEG C by preheater, and the inlet tube 1 through bottom inputs micro- logical
Road reactor, hydrogen source material is uniformly distributed by the inlet opening 2 on inlet tube 1 enters what each gap by between substrate 3 formed
Microchannel, on the catalyst coat in microchannel, hydrogen source material is broken down into hydrogen storage carrier and hydrogen, and product goes out from microchannel
Mouthful enter gas-liquid separation chamber 4, under the effect of gravity, hydrogen storage carrier flow downward through outlet tube 6 be discharged reactor, hydrogen rise by
Reactor is discharged in escape pipe 5.
The above embodiment is a preferred embodiment of the present invention, but embodiments of the present invention are not by above-described embodiment
Limitation, other any changes made without departing from the spirit and principles of the present invention, modification, alternative combinations and simplification,
It should be equivalent substitute mode, be included within the scope of the present invention.
Claims (10)
1. a kind of micro passage reaction of the dehydrogenation reaction suitable for liquid hydrogen source material, which is characterized in that the microchannel plate
Answer device cylindrical, including outer wall, inlet tube, substrate, gas-liquid separation chamber, outlet tube and escape pipe；It is offered on the inlet tube
Several inlet openings are connect upwardly through the inlet opening with the substrate, on the substrate in the Vertical Square of the inlet tube
It is coated with catalyst coat, the substrate is divided into sector by several deflectors and forms, and electric heating wire is provided in the substrate, described
It is provided with flow-disturbing point on substrate, forms microchannel between the substrate, the gas-liquid separation chamber is the substrate and the outer wall
Between region, the escape pipe is located at the top of the micro passage reaction, and the outlet tube is located at micro passage reaction
Bottom, the outer wall coat thermal insulation material.
2. the micro passage reaction of the dehydrogenation reaction according to claim 1 suitable for liquid hydrogen source material, feature exist
In the number of the substrate is 2~1000, and the shape of the substrate is one or more of straight panel, wave-shape board or folded plate, institute
The number for stating deflector is 2~32, and the diameter of the substrate is 0.1~0.9 times of the micro passage reaction diameter.
3. the micro passage reaction of the dehydrogenation reaction according to claim 1 suitable for liquid hydrogen source material, feature exist
In the thermal insulation material is one or more of glass fibre, polyurethane, rock wool, pearlife or aeroge.
4. the micro passage reaction of the dehydrogenation reaction according to claim 1 suitable for liquid hydrogen source material, feature exist
In the flow-disturbing point is circular protrusions or square protrusion.
5. the micro passage reaction of the dehydrogenation reaction according to claim 1 suitable for liquid hydrogen source material, feature exist
In, the microchannel with a thickness of 50~2000 microns.
6. the micro passage reaction of the dehydrogenation reaction according to claim 1 suitable for liquid hydrogen source material, feature exist
In the catalyst coat is metal layer, and the metal layer is first to coat AlOOH sol layer on substrate, is generated by calcining I
γ-Al2O3Coating, then again in γ-Al2O3Metal salt is coated on coating as presoma, in air or inert atmosphere
Under, metal oxide is obtained by calcining II, in a hydrogen atmosphere, reduction reaction is carried out and is made.
7. the micro passage reaction of the dehydrogenation reaction according to claim 6 suitable for liquid hydrogen source material, feature exist
In the metal layer is one or more of Pt, Rh, Ru, Pd, Ni, Co, Mg, Ca or Fe, and the metal salt is above-mentioned metal
Nitrate, acetate, oxalates, carbonate, bicarbonate, sulfate or chloride, the inert atmosphere are N2, Ar or He；
The temperature of the calcining I is 300~600 DEG C, and the temperature of the calcining II is 200~550 DEG C, and the temperature of the reduction reaction is
200~500 DEG C；The calcining I and calcining II, the time of reduction reaction is 3~8h, the metal layer, γ-Al2O3Coating,
The thickness of metal salt is 10~100 microns.
8. the micro passage reaction of the dehydrogenation reaction according to claim 1-7 suitable for liquid hydrogen source material
Method of dehydrogenating, which is characterized in that the specific steps of which are as follows:
S1. the preheated device of hydrogen source material is preheated to 80~300 DEG C, and the inlet tube through bottom inputs micro passage reaction, hydrogen source material
Material is uniformly distributed by the inlet opening on inlet tube into the microchannel being made of the gap between substrate；
S2. on the catalyst coat in microchannel, hydrogen source material is broken down into hydrogen storage carrier and hydrogen, and product goes out from microchannel
Mouthful enter gas-liquid separation chamber, under the effect of gravity, hydrogen storage carrier, which flows downward, is discharged micro passage reaction through outlet tube, on hydrogen
It rises and micro passage reaction is discharged by escape pipe, complete Dehydroepiandrosterone derivative.
9. the dehydrogenation side of the micro passage reaction of the dehydrogenation reaction according to claim 8 suitable for liquid hydrogen source material
Method, which is characterized in that hydrogen storage carrier described in step S2 is in unsaturated arene compound and/or heterocycle unsaturated compound
One or more mixtures with solvent, the unsaturation arene compound and/or heterocycle unsaturated compound: solvent
Mass ratio is (0.03~0.97): 1.
10. the dehydrogenation side of the micro passage reaction of the dehydrogenation reaction according to claim 9 suitable for liquid hydrogen source material
Method, which is characterized in that it is described unsaturation arene compound be benzene, toluene, ethylbenzene, propyl benzene, isopropylbenzene, ortho-xylene, to two
Toluene, meta-xylene, styrene, naphthalene, anthracene, phenanthrene, phenol, aniline and its substance described above derivative；The heterocycle insatiable hunger
It is carbazole, indoles, N- methyl carbazole, N- ethyl carbazole, N- n-propyl carbazole, N- isopropylcarbazole, N- normal-butyl with compound
Carbazole, N- methyl indol, N- ethylindole, pyrazine, furans, pyrroles, thiazole, pyridine, penta pyrazine of ring, benzothiazole and its derivative
Object；The solvent be methanol, ethyl alcohol, isopropanol, ethylene glycol, normal propyl alcohol, n-butanol, ether, methyl ether, acetonitrile, formic acid, acetic acid,
Ethyl acetate, methyl acetate, Ethyl formate, n-butyl ether, isopropyl ether, methylene chloride, chloroform, tetrachloromethane, dichloroethanes, just oneself
One or more of alkane, hexamethylene, pentane, normal octane, carbon disulfide or petroleum ether.
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