CN103552982A - Sodium borohydride hydrolysis/alcoholysis hydrogen production reactor - Google Patents
Sodium borohydride hydrolysis/alcoholysis hydrogen production reactor Download PDFInfo
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- CN103552982A CN103552982A CN201310587007.3A CN201310587007A CN103552982A CN 103552982 A CN103552982 A CN 103552982A CN 201310587007 A CN201310587007 A CN 201310587007A CN 103552982 A CN103552982 A CN 103552982A
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- hydrogen
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- sodium borohydride
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- 239000001257 hydrogen Substances 0.000 title claims abstract description 49
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 49
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 47
- 239000012279 sodium borohydride Substances 0.000 title claims abstract description 26
- 229910000033 sodium borohydride Inorganic materials 0.000 title claims abstract description 26
- 238000004519 manufacturing process Methods 0.000 title claims abstract description 23
- 238000006136 alcoholysis reaction Methods 0.000 title claims abstract description 11
- 238000006460 hydrolysis reaction Methods 0.000 title claims abstract description 11
- 230000007062 hydrolysis Effects 0.000 title claims abstract description 10
- 238000006243 chemical reaction Methods 0.000 claims abstract description 51
- 239000002994 raw material Substances 0.000 claims abstract description 23
- 239000007788 liquid Substances 0.000 claims abstract description 18
- 239000007789 gas Substances 0.000 claims abstract description 15
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 11
- 229910000510 noble metal Inorganic materials 0.000 claims abstract description 5
- 238000010276 construction Methods 0.000 claims description 4
- 229910052878 cordierite Inorganic materials 0.000 claims description 3
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 claims description 3
- 239000008187 granular material Substances 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 230000008649 adaptation response Effects 0.000 claims 1
- 229910052763 palladium Inorganic materials 0.000 claims 1
- 229910052697 platinum Inorganic materials 0.000 claims 1
- 239000010970 precious metal Substances 0.000 claims 1
- 229910052703 rhodium Inorganic materials 0.000 claims 1
- 229910052707 ruthenium Inorganic materials 0.000 claims 1
- 239000000047 product Substances 0.000 abstract description 6
- 238000000926 separation method Methods 0.000 abstract description 6
- 239000003054 catalyst Substances 0.000 abstract description 5
- 230000007613 environmental effect Effects 0.000 abstract description 3
- 229910052799 carbon Inorganic materials 0.000 abstract 1
- 239000012263 liquid product Substances 0.000 abstract 1
- 239000002923 metal particle Substances 0.000 abstract 1
- 239000000446 fuel Substances 0.000 description 13
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 9
- 238000003860 storage Methods 0.000 description 8
- 238000000034 method Methods 0.000 description 6
- 239000000243 solution Substances 0.000 description 6
- 239000006227 byproduct Substances 0.000 description 5
- 239000000463 material Substances 0.000 description 4
- 238000011160 research Methods 0.000 description 4
- NVIFVTYDZMXWGX-UHFFFAOYSA-N sodium metaborate Chemical compound [Na+].[O-]B=O NVIFVTYDZMXWGX-UHFFFAOYSA-N 0.000 description 4
- 239000007864 aqueous solution Substances 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 2
- 230000003197 catalytic effect Effects 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 150000002431 hydrogen Chemical class 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 239000011232 storage material Substances 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000008014 freezing Effects 0.000 description 1
- 238000007710 freezing Methods 0.000 description 1
- OAKJQQAXSVQMHS-UHFFFAOYSA-N hydrazine Substances NN OAKJQQAXSVQMHS-UHFFFAOYSA-N 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 230000003301 hydrolyzing effect Effects 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 230000000977 initiatory effect Effects 0.000 description 1
- 230000010354 integration Effects 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Images
Classifications
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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
- 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
Abstract
The invention relates to a sodium borohydride hydrolysis/alcoholysis hydrogen production reactor. The main body of the reactor has a double-layer sleeve structure, wherein the inner layer is a reaction chamber and the outer layer comprises a raw material chamber and a gas/liquid separation chamber. The raw material chamber consists of an upper part and a lower part which are communicated with each other through a tube bundle with a deflection baffle, and the space outside the tube bundle serves as the gas/liquid separation chamber. Reaction raw materials from the nether raw material chamber are input into the reaction chamber by a hydraulic pump and enter a catalyst bed layer through a distribution plate. The catalyst bed layer of the reaction chamber is divided into an upper section and a lower section, wherein the upper section is active carbon loaded with a noble metal particles, and the lower section is an overall structure catalyst. A product leaving the reaction chamber enters the gas/liquid separation chamber, and exchanges heat with the raw materials in the tube bundle through a pipe wall to ensure that the raw materials can be preheated, and the separation of hydrogen and a liquid product is realized at the same time. According to the sodium borohydride hydrolysis/alcoholysis hydrogen production reactor, the sodium borohydride hydrolysis/alcoholysis hydrogen production reaction can be performed under a natural condition; the reactor is compact in structure, integrates reaction, heat exchange and product separation, and can meet requirements for real-time hydrogen production under various environmental conditions.
Description
Technical field
The present invention relates to a kind of reactor that utilizes catalyzer and sodium borohydride to produce hydrogen, can meet the needs of instant hydrogen manufacturing at various varying environment temperature.
Background technology
Hydrogen Energy is regarded as 21 century the most potential clean energy and energy carrier.In recent years, the Hydrogen Energy development and utilization that the fuel cell technology of take is representative is subject to the great attention of countries in the world, and commercialization is realized in beginning.Wherein, Proton Exchange Membrane Fuel Cells is considered to the third generation power system after steamer and oil engine, in fields such as stationary electric power plant, power truck, military special type power supply, movable power sources, has broad application prospects.
Proton Exchange Membrane Fuel Cells is used pure hydrogen as fuel, but existing hydrogen storage material and technology are at aspects such as quality and volume hydrogen-storage density, working temperature, reversible cycle performance and securities, can't meet practical and requirement mass-producing.Therefore, adopting hydrogen-rich fuel to carry out situ conversion, to prepare the method for hydrogen be the effective means that meets the practical needs of fuel cell present stage.
In recent years, hydroborate sodium borohydride (NaBH particularly
4) as novel hydrogen storage material, be subject to extensive concern.High temperature reformation hydrogen production reacting phase ratio with hydro carbons and alcohols, sodium borohydride catalyzing hydrolyzation reaction can be carried out at normal temperatures, do not need additionally to provide energy to carry out initiation reaction, reaction liberated heat can maintain reaction to carry out with speed faster under self-heat condition, easily realizes instant hydrogen manufacturing and instant hydrogen supply.In addition, in prepared hydrogen, not containing CO and other impurity, can be directly used in fuel cell, moisture contained in hydrogen can also play the effect to fuel battery proton exchange film humidification.
The alcoholysis reaction of sodium borohydride and methyl alcohol can be carried out at 0 ℃ of even lower temperature.It is that sodium borohydride alcoholysis hydrogen production process can be applied under extremely cold environment that the freezing point of methyl alcohol is-97 ℃, has greatly expanded the environmental compatibility of sodium borohydride hydrogen manufacturing.
With regard to preparing hydrogen by sodium borohydride hydrolysis practical, generally need to adopt flow reactor, this just require raw material sodium borohydride and by product sodium metaborate completely soluble in water.Yet sodium borohydride hydrolysising by-product sodium metaborate is with the form stable existence of hydrate.At 25 ℃, guarantee sodium metaborate is in solution state during only lower than 28g/100g water for the concentration of sodium borohydride in the aqueous solution, and at this moment the weight hydrogen-storage density of system only has 2.9wt%.The quality hydrogen-storage density that USDOE has proposed following medium-term and long-term target: 2005-2010 to the vehicle-mounted hydrogen storage system of fuel cell car reaches 6.5%, and volume hydrogen-storage density reaches 62kg/m
3; The quality hydrogen-storage density of 2015 reaches 9%, and volume hydrogen-storage density reaches 80kg/m
3.Therefore, sodium borohydride hydrolysis reaction system is also not suitable for use in the hydrogen-feeding system of on-vehicle fuel, but the method still has potential application prospect at portable electric source domain.
In sum, although be subject to raw materials cost and hydrogen-storage density restriction, the hydrogen production process that the hydroborate of take is raw material is still suitable at varying environment temperature, as portable fuel battery provides instant hydrogen manufacturing and hydrogen supply, having become the focus of fuel cell hydrogen source area research and exploitation.From research report and patent content, the research of this method is focused mostly in catalyzer and reaction kinetics, but less for the research report of reactor.
Chinese patent (CN101049907B) has been announced a kind of method and device of instant self-controlled hydrogen supply of chemical borohydride hydrolytic hydrogen production.The method is the poor effect of hydrogen pressure between inner two encloses containers of use device, makes to flow between two containers of reaction material in device, regulates the Exposure of reaction material and catalyzer, thereby controls generation speed and the pressure of hydrogen.This apparatus structure is simple, can realize instant hydrogen supply.Chinese patent (CN100560477C) has been announced a kind of preparation method of tubular reactor of hydrogen production by sodium borohydride-hydrazine mixed fuel, metal support after dealuminzation is packed into tubular reactor as catalyzer, can realizes continuous hydrogen supply and with stable speed hydrogen supply.But the reactor function singleness in existing method and apparatus, and not for reaction characteristics design bed structure and the management of consideration reaction heat.
Summary of the invention
The invention provides a kind of sodium borohydride hydrolysis/alcoholysis hydrogen-manufacturing reactor.This reactor can improve the compactness of reactor; Reduce the start time of reacting under envrionment temperature; Reduce the resistance to mass transfer of the material in beds, improve reaction efficiency.
To achieve these goals, reactor body provided by the invention is partly double-layer sleeve structure, is from inside to outside followed successively by reaction chamber and feed chamber.Wherein, feed chamber by upper (12), under (18) two portions form, and be connected by built-in tube bank (4), the space outside tube bank is as gas/liquid separate chamber (8).
After reaction starts, utilize small-scale liquid press pump (1) that reaction raw materials is extracted out and is transported to reaction chamber entrance (10) through pipeline (7) by below feed chamber outlet (2), the under meter on pipeline 7 (5) is in order to measure reaction raw materials.Reaction chamber beds forms by upper and lower two sections.Epimere is activated carbon supported noble metal granule catalyzer (14), and hypomere is one-piece construction catalyzer (16).In two-stage catalytic agent layer upper end, there are respectively grid distributor 9 and 6.The product that leaves reaction chamber enters gas/liquid separate chamber through check valve (17), this with tube bank in raw material counter-current flow, by tube wall and its heat exchange, make raw material obtain preheating, realize the separated of hydrogen and product liquid simultaneously.For improving heat exchange efficiency, baffle plate (3) is housed on tube wall in gas/liquid separate chamber.
Native system can carry out under self-heat condition.When reaction raw materials enters in reactor, need certain start time and just can reach stable hydrogen output.Be subject to the impact of envrionment temperature, have certain fluctuation start time.Under autothermal reaction condition, in order to reduce start time, at reaction chamber epimere, load activated carbon supported noble metal granule catalyzer, guarantee that reaction carries out with speed faster at ambient temperature.
Most of reactant completes conversion at reaction chamber epimere, and for sodium borohydride aqueous solution system, by product sodium metaborate is that along with the consumption of water in reaction process, system viscosity increases, mobility variation with the form stable existence of hydrate.For avoiding reaction chamber to stop up, at reaction chamber hypomere, adopt honeycomb integral catalyst, improve the mobility of product solution, complete the conversion of residue sodium borohydride simultaneously.
Hydrogen after separation is left by the top outlet (13) of gas/liquid separate chamber, and by-product solution is discharged by the centre exit (15) of gas/liquid separate chamber.
Compared with prior art, advantage of the present invention and positively effect are:
One, by reaction chamber, Heat Room and the integrated reactor of gas/liquid separate chamber effective integration, improved the compactness of reactor, small volume, can meet the instant hydrogen manufacturing needs of miniaturization;
Two, for reaction characteristics, constructed upper and lower two-stage catalytic agent bed.Epimere adopts high reactivity noble metal support catalyzer, and hypomere adopts honeycomb integral catalyst.Both meet the requirement that reaction starts fast, overcome again the reaction later stage because soltion viscosity increase causes the problem that in beds, resistance to mass transfer increases;
Three, the heat exchange by product and raw material raises material temperature, is conducive to shorten react start time, meets the needs of instant hydrogen manufacturing under cold environmental conditions;
Four, reaction product is by with raw material heat exchange and arrange plate washer, strengthened the separated of hydrogen and product solution.
Accompanying drawing explanation
Fig. 1 is sodium borohydride hydrolysis/alcoholysis hydrogen-manufacturing reactor schematic diagram of the present invention.
Fig. 2 is baffle schematic diagram in sodium borohydride hydrolysis/alcoholysis hydrogen-manufacturing reactor gas/liquid of the present invention separate chamber.
Embodiment
Below in conjunction with the drawings and specific embodiments, technical scheme of the present invention is described in further detail, the present invention is not limited to these embodiment.
Embodiment 1
According to the sodium borohydride hydrogen making reaction device shown in Fig. 1, beds epimere is activated carbon supported Pt catalyzer, and hypomere is that honeycomb cordierite supports Co and Ni one-piece construction catalyzer.Adopting sodium borohydride and naoh concentration to be respectively 10% and 5% the aqueous solution is raw material, and (20 ℃) carry out instant hydrogen manufacturing at ambient temperature, and the flow velocity of reaction raw materials is 20ml/min, and it is 5L/min that reaction reaches the hydrogen flow rate producing after steady state.
Embodiment 2
According to the sodium borohydride hydrogen making reaction device shown in Fig. 1, beds epimere is activated carbon supported Pt catalyzer, and hypomere is that honeycomb cordierite supports Co and Ni one-piece construction catalyzer.Adopting sodium borohydride and naoh concentration to be respectively 5% and 2% methanol solution is raw material, under outdoor conditions, (0 ℃ of left and right) carries out instant hydrogen manufacturing in the winter time, the flow velocity of reaction raw materials is 20ml/min, and it is 2.4L/min that reaction reaches the hydrogen flow rate producing after steady state.
Above embodiment is only in order to technical scheme of the present invention to be described, but not is limited; Although the present invention is had been described in detail with reference to previous embodiment, for the person of ordinary skill of the art, the technical scheme that still can record previous embodiment is modified, or part technical characterictic is wherein equal to replacement; And these modifications or replacement do not make the essence of appropriate technical solution depart from the spirit and scope of the present invention's technical scheme required for protection.
Claims (3)
1. a sodium borohydride hydrolysis/alcoholysis hydrogen-manufacturing reactor, main part is tube-in-tube structure, and internal layer is reaction chamber, and skin is feed chamber and gas/liquid separate chamber.Feed chamber is comprised of upper and lower two portions, and is connected by built-in tube bank, and the space outside tube bank is as gas/liquid separate chamber.
Reaction raw materials from below feed chamber pumps into reaction chamber after metering.Reaction chamber beds forms by upper and lower two sections.The product that leaves reaction chamber enters gas/liquid separate chamber through check valve, this with tube bank in raw material counter-current flow, by tube wall and its heat exchange, make raw material obtain preheating, realize the separated of hydrogen and product liquid simultaneously.
2. reactor according to claim 1, restrains outer wall with baffle plate in gas/liquid separate chamber, and feed chamber and gas/liquid separate chamber form tube and shell heat exchanger.
3. reactor according to claim 1, reaction chamber beds epimere is activated carbon supported noble metal granule catalyzer, to meet, realizes the requirement starting fast under lower envrionment temperature, precious metal is one or more in Pt, Pd, Rh, Ru; Hypomere is that honeycomb cordierite supports Co and Ni one-piece construction catalyzer, the situation of the mobility variation cause because soltion viscosity increases with the adaptive response later stage.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201310587007.3A CN103552982B (en) | 2013-11-20 | 2013-11-20 | Sodium borohydride hydrolysis/alcoholysis hydrogen production reactor |
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| Application Number | Priority Date | Filing Date | Title |
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| CN201310587007.3A CN103552982B (en) | 2013-11-20 | 2013-11-20 | Sodium borohydride hydrolysis/alcoholysis hydrogen production reactor |
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| CN103552982A true CN103552982A (en) | 2014-02-05 |
| CN103552982B CN103552982B (en) | 2015-07-01 |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108862191A (en) * | 2018-08-16 | 2018-11-23 | 深圳亚华伟翌科技有限公司 | Sodium borohydride hydrolysis hydrogen production unit |
| CN110550599A (en) * | 2018-05-31 | 2019-12-10 | 吉林大学 | Hydrolysis hydrogen production system |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2007084142A2 (en) * | 2005-01-28 | 2007-07-26 | Millennium Cell, Inc. | Hydrogen generation system and method |
| CN101027247A (en) * | 2004-06-14 | 2007-08-29 | 千年电池公司 | Catalytic reactor for hydrogen generation systems |
| CN101054160A (en) * | 2006-04-10 | 2007-10-17 | 中国科学院大连化学物理研究所 | Mini reforming hydrogen-preparation reactor |
| CN101597023A (en) * | 2008-06-03 | 2009-12-09 | 中国科学院金属研究所 | Be applicable to the chemical hydride catalytic-hydrolysis device for producing hydrogen and the method for onboard hydrogen source |
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2013
- 2013-11-20 CN CN201310587007.3A patent/CN103552982B/en not_active Expired - Fee Related
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101027247A (en) * | 2004-06-14 | 2007-08-29 | 千年电池公司 | Catalytic reactor for hydrogen generation systems |
| WO2007084142A2 (en) * | 2005-01-28 | 2007-07-26 | Millennium Cell, Inc. | Hydrogen generation system and method |
| CN101054160A (en) * | 2006-04-10 | 2007-10-17 | 中国科学院大连化学物理研究所 | Mini reforming hydrogen-preparation reactor |
| CN101597023A (en) * | 2008-06-03 | 2009-12-09 | 中国科学院金属研究所 | Be applicable to the chemical hydride catalytic-hydrolysis device for producing hydrogen and the method for onboard hydrogen source |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110550599A (en) * | 2018-05-31 | 2019-12-10 | 吉林大学 | Hydrolysis hydrogen production system |
| CN108862191A (en) * | 2018-08-16 | 2018-11-23 | 深圳亚华伟翌科技有限公司 | Sodium borohydride hydrolysis hydrogen production unit |
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| CN103552982B (en) | 2015-07-01 |
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