CN103303864A - Method and device for preparing hydrogen by hydrolysis of hydroboron, and application - Google Patents
Method and device for preparing hydrogen by hydrolysis of hydroboron, and application Download PDFInfo
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- CN103303864A CN103303864A CN2013102472638A CN201310247263A CN103303864A CN 103303864 A CN103303864 A CN 103303864A CN 2013102472638 A CN2013102472638 A CN 2013102472638A CN 201310247263 A CN201310247263 A CN 201310247263A CN 103303864 A CN103303864 A CN 103303864A
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- 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
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Abstract
The invention provides a method and a device for preparing hydrogen by hydrolysis of hydroboron, and an application. The method comprises the steps of preparing hydrogen by hydrolysis of hydroboron under an alkaline condition; loading metal cobalt and metal cerium or zirconium to a molecular sieve as a bimetallic catalyst; and adding urea as a reaction stabilizer. By adopting the method and the device, hydrogen production by hydrolysis of hydroboron known at present is selected as an efficient hydrogen production system; a novel stabilizer is added to control the intense degree of the reaction and keep the hydrogen production rate stable; the reaction is more efficient by adopting a homemade catalyst; and simple purification is carried out in a hydrogen collection process. The hydrogen production method can be directly applied to a miniature fuel cell with certain powder; and extra storage, purification and drying devices are not needed.
Description
Technical field
The invention belongs to clean energy and utilize the field, relate to the preparation method of hydrogen, relate in particular to method, device and application that a kind of borohydride hydrolytic prepares hydrogen.
Background technology
In recent years, along with the exhaustion of society and development of science and technology and fossil oil, new energy developments such as hydrogen have become the research focus.The key areas that Proton Exchange Membrane Fuel Cells is used as hydrogen energy source receives much concern always, at present, is also obtaining bigger progress aspect the research of big-and-middle-sized fuel cells such as automobile-used Proton Exchange Membrane Fuel Cells.But along with the needs of special dimension to small fuel cell, the fuel cell miniaturization becomes problem demanding prompt solution gradually.Mostly be high-pressure hydrogen storing at present the method for fuel cell supply of hydrogen, but this is for the limited small fuel cell of hydrogen amount, it is huge, complicated, inconvenient that high-pressure hydrogen storing equipment just shows, therefore, exploitation a kind of rationally, steadily, can direct applied hydrogen production process be the key that solves the supply of miniaturization fuel cell hydrogen.
In addition, existing hydroborate catalysis is produced in the method for hydrogen, is purpose with high-speed, high purity, the controllability of pursuing that hydrogen produces mostly, and expectation can produce the high-purity hydrogen of capacity within a short period of time, and its storage is used.At present in the disclosed relevant patent, seldom relate to and how to take effective means to make hydrogen-producing speed become more steady satisfying under the condition of particular demands.In the compact pem fuel cell field, because its output rating limited (2W-50W), the hydrogen supply speed that needs is not high, even under some special conditions, there is not hydrogen to store and the purification means, therefore, exploitation is a kind of just seems particularly important for the hydrogen production process of the instant hydrogen supply of small fuel cell.
Summary of the invention
The object of the invention is to overcome the prior art defective, provides a kind of preparation hydrogen process steady, and gas production rate is controlled, and the simple borohydride hydrolytic of reaction unit prepares method and the device of hydrogen.
Borohydride hydrolytic prepares the method for hydrogen, and borohydride hydrolytic prepares hydrogen under alkaline condition, is carried on molecular sieve as bimetallic catalyst with base metal, adds urea as reaction stabilizer.
Described bimetallic catalyst reactive metal is cobalt, and helping catalytic metal is a kind of in cerium or the zirconium.
Described hydroborate is sodium borohydride, POTASSIUM BOROHYDRIDE, the one or more combination of lithium borohydride.
Described alkaline condition is by adding wherein one or more the mixture formation in sodium hydroxide, potassium hydroxide, lithium hydroxide, the calcium hydroxide.
Borohydride hydrolytic prepares the device of hydrogen method, comprises three mouthfuls of containers, and three mouthfuls of containers place the constant temperature system, and three mouths of described three mouthfuls of containers are respectively hydrogen outlet, temperature-measuring port and charging opening, and the hydrogen outlet top of three mouthfuls of containers is equipped with the hydrogen filtration unit.
Described hydrogen filtration unit is the Glass tubing that solid super-strong acid is housed, and there is the mouth of pipe that can connect sebific duct at two ends.
Borohydride hydrolytic prepares the application of hydrogen method, and it is the compact pem fuel cell supply of hydrogen of certain power directly that this method is used for.
Compared with prior art, advantage of the present invention is as follows:
(1) stablizer that adds in this method is urea, does not still have the report that urea is used in this regard at present, has certain originality.The interpolation of urea is reacted severe degree for slowing down, steadily hydrogen-producing speed has remarkable effect.
(2) this method is emphasized under the situation that satisfies compact pem fuel cell hydrogen supply speed needs hydrogen at the uniform velocity to be produced, and according to the hydrogen demand speed of the small fuel cell of different output power, directly is its hydrogen supply.
(3) hydrogen of this method preparation does not need storage, deep purifying and drying, only remove the small amount of alkali mist and can directly utilize by the simple hydrogen gas filtration unit is set, and the hydrogen that utilizes the inventive method to prepare has certain humidity, and fuel battery proton exchange film is had certain wetting action.
(4) this method application is fixed (compact pem fuel cell), not simple high-speed, the high purity of pursuing Preparation of Hydrogen, and emphasis provides can direct applied hydrogen supply technology in the proton exchanging film fuel battery miniaturization process.
(5) material cost such as related catalyzer (base metal bimetallic catalyst), stablizer is low in this method, and economy is obvious.
Description of drawings
Fig. 1 is apparatus of the present invention structural representations.
Fig. 2 is that experimental example 1 and experimental example 2 produce the hydrogen effect contrast figure;
Fig. 3 is that experimental example 3 produces the hydrogen design sketch.
Embodiment
For making the purpose, technical solutions and advantages of the present invention clearer, below in conjunction with the accompanying drawing among the present invention, the technical scheme among the present invention is clearly and completely described, obviously, described embodiment is the present invention's part embodiment, rather than whole embodiment.Based on the embodiment among the present invention, those of ordinary skills belong to the scope of protection of the invention not making the every other embodiment that obtains under the creative work prerequisite.
Fig. 1 is apparatus of the present invention structural representations, as shown in Figure 1, borohydride hydrolytic prepares the device of hydrogen method, this device comprises three mouthfuls of container there-necked flasks, three mouthfuls of containers place the constant temperature system, the constant temperature system is made up of Water Tank with Temp.-controlled 8 and automatic temp controller 1, and three mouths of there-necked flask are respectively on the hydrogen outlet 3 of hydrogen outlet 3, temperature-measuring port 4 and 5, three mouthfuls of containers of charging opening hydrogen filtration unit 2 and gas meter 9 are installed.
Borohydride hydrolytic prepares the method embodiment of hydrogen:
Embodiment 1:
Use an amount of NaBH
4, the NaOH obtain solution is as reaction solution, is carried on molecular sieve as bimetallic catalyst with cobalt metal and metallic cerium, add a certain amount of urea and produce hydrogen as reaction stabilizer.
Embodiment 2:
Use an amount of KBH
4, the NaOH obtain solution is as reaction solution, is carried on molecular sieve as bimetallic catalyst with cobalt metal and metallic cerium, add a certain amount of urea and produce hydrogen as reaction stabilizer.
Embodiment 3:
Use an amount of KaBH
4, NaBH
4, the NaOH obtain solution is as reaction solution, is carried on molecular sieve as bimetallic catalyst with cobalt metal and metallic cerium, add a certain amount of urea and produce hydrogen as reaction stabilizer.
Embodiment 4:
Use an amount of NaBH
4, NaOH, KaOH obtain solution be as reaction solution, is carried on molecular sieve as bimetallic catalyst with cobalt metal and metal zirconium, add a certain amount of urea and produce hydrogen as reaction stabilizer.
Experimental example 1:
(1) according to the experimental installation of building shown in Figure 1, there-necked flask is placed Water Tank with Temp.-controlled 8, connect hydrogen outlet 3, hydrogen filtration unit 2, wet test meter 9 with sebific duct successively from top to bottom, hydrogen outlet 3 and temperature-measuring port 4 use the soft rubber ball sealing that is inserted with Glass tubing and thermometer respectively;
(2) use an amount of NaBH
4, the NaOH obtain solution is as reaction solution 6, from charging opening 5 solution added there-necked flask, regulate automatic temp controller 1 and make the constant temperature system be stabilized in specified temp;
(3) from charging opening 5 catalyzer 7 is added reaction solution 6 rapidly, with charging opening 5 sealings, pick up counting simultaneously (hydrogen generating quantity of the identical time record in every interval) stops timing and mapping after product hydrogen finishes with the soft rubber ball sealing.In actual applications, hydrogen produces and is supplied to compact pem fuel cell by hydrogen outlet 3, simple hydrogen gas filtration unit 2 and sebific duct successively.
Experimental example 2:
(1) according to the experimental installation of building shown in Figure 1, there-necked flask is placed constant temperature system 8, connect hydrogen outlet 3, simple hydrogen gas filtration unit 2, wet test meter 9 with sebific duct successively from top to bottom, the middle soft rubber ball sealing that is inserted with Glass tubing and thermometer respectively of hydrogen outlet 3 and temperature-measuring port 4 usefulness;
(2) use an amount of NaBH
4, NaOH, urea obtain solution be as reaction solution 6, from charging opening 5 solution added there-necked flask, regulate automatic temp controller 1 and make the constant temperature system be stabilized in specified temp;
(3) from charging opening 5 catalyzer 7 is added reaction solution 6 rapidly, with charging opening 5 sealings, pick up counting simultaneously (each identical time record is amounts of hydrogen successively) stops timing and mapping after product hydrogen finishes with the soft rubber ball sealing;
This experimental example is that with unique difference of experimental example 1 reaction solution 6 that experimental example 1 is prepared only contains an amount of NaBH
4, NaOH, do not add urea.
Fig. 2 is that experimental example 1 and experimental example 2 produce the hydrogen effect contrast figure, as shown in Figure 2, after the interpolation stablizer adds in this hydrogen production process, totally produce hydrogen speed and descend to some extent, but produce the hydrogen kinetic curve near straight line, hydrogen-producing speed is constant substantially, and (the average hydrogen-producing speed difference of adjacent per minute is not more than 0.05Lmin
-1), hydrogen-producing speed maintains 0.12Lmin
-1About, can supply output rating and be the small fuel cell continued running about 20W.
Experimental example 3:
(1) with an amount of NaBH
4, NaOH, urea preparation reaction solution, make urea concentration be respectively 5g/L, 10g/L, 15g/L (be calculating standard with the overall solution volume);
(2) select the solution that contains the different concns stablizer respectively for use, step in the repeated experiments example 2 (1)-(3).
Fig. 3 is that experimental example 3 produces the hydrogen design sketch, as can be seen from Figure 3, the stablizer of different concns has remarkably influenced to the generation of hydrogen, the stablizer add-on is more big, average hydrogen-producing speed descends more many, but produce the hydrogen kinetic curve all near straight line, hydrogen-producing speed is constant substantially, can satisfy the hydrogen supply needs of the small fuel cell of different output power by control stablizer add-on.
The present invention relates to hydrogen production process, NaBH
4The research of hydrolytic hydrogen production belongs to the clean energy Application Areas, and a kind of novel steady hydrogen production process, device and application are provided especially.This method is utilized as starting point with hydrogen energy source, and emphasis solves the direct hydrogen supply problem of small-sized proton exchange membrane hydrogen-oxygen fuel cell, and realization is produced hydrogen and carried out simultaneously with hydrogen.Hydrogen output speed with the inventive method preparation is steady, do not need extra storage, purification means just can be directly used in small fuel cell, in the direct hydrogen supply of small fuel cell field, particularly under the prerequisite of hydrogen storage, purification condition deficiency, the present invention has vast market prospect.
Borohydride hydrolytic provided by the invention prepares method, device and the application of hydrogen, this method utilizes the alkaline condition borohydride hydrolytic to prepare hydrogen, advancing reaction by interpolation self-control bimetallic catalyst short (cobalt metal and metallic cerium or zirconium) carries out, adding a kind of novel reaction stablizer is urea, make hydrogen-producing speed satisfy under the prerequisite of specific needs more steady.Hydrogen production reaction carries out in three mouthfuls of containers, hydrogen is collected from the centre outlet, two side outlets are respectively applied to the assaying reaction liquid temp and material adds, central exit top is provided with the simple hydrogen gas filtration unit, this method can be directly used in the supply of compact pem fuel cell hydrogen under the condition that does not have hydrogen storage and additional purification means.
The affiliation that adds of stablizer obviously reduces the reaction severe degree among the present invention, and the average hydrogen-producing speed difference of steady, the adjacent per minute of hydrogen-producing speed is not more than 0.05Lmin
-1Bimetallic catalyst of the present invention is loaded catalyst, and carrier is molecular sieve, does not contain precious metal (example: gold and silver, platinum, ruthenium, rhodium, palladium etc.) in the catalyzer.
Described hydrogen filtration unit is the Glass tubing that solid super-strong acid is housed, and there is the mouth of pipe that can connect sebific duct at two ends, makes simple.
It is 2W-50W that the present invention is used for the compact pem fuel cell output rating of hydrogen is provided.
The speed of reaction of hydrogen of the present invention can realize by the following variable of control: (1) catalyst consumption; (2) concentration of hydroborate and alkali; (3) consumption of stablizer.
The innovative point of maximum of the present invention is that to have added urea in reaction system be stablizer, cooperates the homemade catalyzer of patent applicant, makes the present invention have the hydrogen of producing characteristics stably.Just because of the present invention has the hydrogen of producing advantage stably, the hydrogen-producing speed that present method has is enough to satisfy the hydrogen supply demand of the compact pem fuel cell of certain power, and can be directly used in compact pem fuel cell, simultaneously, utilize the hydrogen purity height of this method preparation, easy hydrogen filter plant can satisfy the purification requirement of the hydrogen of direct use in the use device, has simplified compact pem fuel cell hydrogen supply equipment greatly.
It should be noted that at last: above embodiment only in order to technical scheme of the present invention to be described, is not intended to limit; Although with reference to previous embodiment the present invention is had been described in detail, those of ordinary skill in the art is to be understood that: it still can be made amendment to the technical scheme that aforementioned each embodiment puts down in writing, and perhaps part technical characterictic wherein is equal to replacement; And these modifications or replacement do not make the essence of appropriate technical solution break away from the spirit and scope of various embodiments of the present invention technical scheme.
Claims (7)
1. borohydride hydrolytic prepares the method for hydrogen, it is characterized in that: borohydride hydrolytic prepares hydrogen under alkaline condition, is carried on molecular sieve as bimetallic catalyst with base metal, adds urea as reaction stabilizer.
2. borohydride hydrolytic as claimed in claim 1 prepares the method for hydrogen, it is characterized in that: described bimetallic catalyst reactive metal is cobalt, and helping catalytic metal is a kind of in cerium or the zirconium.
3. borohydride hydrolytic as claimed in claim 1 prepares the method for hydrogen, it is characterized in that: described hydroborate is sodium borohydride, POTASSIUM BOROHYDRIDE, lithium borohydride one or more combination wherein.
4. borohydride hydrolytic as claimed in claim 1 prepares the method for hydrogen, it is characterized in that: described alkaline condition is by adding wherein one or more the mixture formation in sodium hydroxide, potassium hydroxide, lithium hydroxide, the calcium hydroxide.
One kind according to claim 1 borohydride hydrolytic prepare the device of hydrogen method, it is characterized in that: comprise three mouthfuls of containers, three mouthfuls of containers place the constant temperature system, three mouths of described three mouthfuls of containers are respectively hydrogen outlet (3), temperature-measuring port (4) and charging opening (5), and the hydrogen outlet of three mouthfuls of containers (3) top is equipped with hydrogen filtration unit (2).
6. borohydride hydrolytic as claimed in claim 5 prepares the device of hydrogen method, it is characterized in that: described hydrogen filtration unit (2) is for being equipped with the Glass tubing of solid super-strong acid, and there is the mouth of pipe that can connect sebific duct at two ends.
7. the borohydride hydrolytic application for preparing the hydrogen method according to claim 1 is characterized in that: this method is used for directly being the compact pem fuel cell supply of hydrogen of certain power.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104891435A (en) * | 2015-05-14 | 2015-09-09 | 大连理工大学 | Hydrogen production method by using proton-responsive iridium complex for catalysis of ammonia borane hydrolysis |
| CN106684406A (en) * | 2017-02-14 | 2017-05-17 | 武汉市能智达科技有限公司 | MgH2 hydrogen-storage material reaction cavity and fuel cell generation device thereof |
| CN109148917A (en) * | 2018-09-13 | 2019-01-04 | 北京化工大学 | A method of realizing that the hydrogen manufacturing of hydrogen storage small molecule exports electric energy simultaneously |
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| CN1911784A (en) * | 2005-08-12 | 2007-02-14 | 比亚迪股份有限公司 | Metal hydrogen compound hydrolysis catalyst for preparing hydrogen and its preparation method and hydrogen producing method using said catalyst |
| CN101100285A (en) * | 2006-07-07 | 2008-01-09 | 中国科学院金属研究所 | Chemical hydride hydrogen storing material system, hydrogen preparing method and hydrogen preparing device |
| CN101587958A (en) * | 2009-07-07 | 2009-11-25 | 重庆大学 | Method for improving performance of direct sodium borohydride fuel cell |
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2013
- 2013-06-21 CN CN2013102472638A patent/CN103303864A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1911784A (en) * | 2005-08-12 | 2007-02-14 | 比亚迪股份有限公司 | Metal hydrogen compound hydrolysis catalyst for preparing hydrogen and its preparation method and hydrogen producing method using said catalyst |
| CN101100285A (en) * | 2006-07-07 | 2008-01-09 | 中国科学院金属研究所 | Chemical hydride hydrogen storing material system, hydrogen preparing method and hydrogen preparing device |
| CN101587958A (en) * | 2009-07-07 | 2009-11-25 | 重庆大学 | Method for improving performance of direct sodium borohydride fuel cell |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104891435A (en) * | 2015-05-14 | 2015-09-09 | 大连理工大学 | Hydrogen production method by using proton-responsive iridium complex for catalysis of ammonia borane hydrolysis |
| CN106684406A (en) * | 2017-02-14 | 2017-05-17 | 武汉市能智达科技有限公司 | MgH2 hydrogen-storage material reaction cavity and fuel cell generation device thereof |
| CN109148917A (en) * | 2018-09-13 | 2019-01-04 | 北京化工大学 | A method of realizing that the hydrogen manufacturing of hydrogen storage small molecule exports electric energy simultaneously |
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Application publication date: 20130918 |