CN103264988A - Method for producing hydrogen by reaction of aluminium and water catalyzed by aluminum hydroxide or oxide - Google Patents
Method for producing hydrogen by reaction of aluminium and water catalyzed by aluminum hydroxide or oxide Download PDFInfo
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- CN103264988A CN103264988A CN2013100753707A CN201310075370A CN103264988A CN 103264988 A CN103264988 A CN 103264988A CN 2013100753707 A CN2013100753707 A CN 2013100753707A CN 201310075370 A CN201310075370 A CN 201310075370A CN 103264988 A CN103264988 A CN 103264988A
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Abstract
The invention provides a method for producing hydrogen by a reaction of aluminium and water catalyzed by aluminum hydroxide or oxides. The invention includes adding a certain amount of (10 wt%-50 wt%) micron or nano-sized aluminum hydroxide or an oxide powder into a closed container containing a certain amount of water, mixing the added aluminum hydroxide or the oxide with water uniformly, adding a certain amount of micron-sized aluminum (Al) directly to the closed container containing the mixture of aluminum hydroxide or the oxide and water, and reacting the pure aluminum (Al) powder with water continuously to produce hydrogen at a temperature of 10 DEG C to 40 DEG C under the vacuum pressure of 0.04 atm to the atmospheric pressure of 1 atm, wherein g-Al2O3 and Al(OH)3 have a good effect on promoting reaction of aluminum (Al) and water to produce hydrogen. Compared with the atmospheric pressure, the speed of reaction of the aluminum powder and water to produce hydrogen is faster under vacuum. The main applications of the invention are hydrogen supplies for mobile kilowatt fuel cells and other small portable fuel cells.
Description
Technical field
The present invention relates to produce with fine aluminium powder and water reaction under a kind of aluminium hydroxide or the oxide compound katalysis processing method of hydrogen, it is a kind of new simple portable product hydrogen methods, can be directly provides hydrogen source for portable multikilowatt fuel cell or the entrained fuel cell of small portable device.The invention belongs to technical field of chemistry and chemical engineering.
Background technology
Along with the concern of people to environmental change, the research and development of high-efficiency cleaning energy technology more and more comes into one's own.Fuel cell is the core of clean energy technology, because fuel cell directly changes chemical energy into electric energy thereby has high efficient and low pollution.Hydrogen is the ideal fuels of fuel cell, be optimum because the oxidation products of hydrogen is water to environment, and hydrogen has characteristics in light weight, that energy density is high.
The significant obstacle that influences the hydrogen fuel cell industrialized development is transportation and the storage of hydrogen.Because liquefying hydrogen needs the low temperature of-252 degrees centigrade (° C), at normal temperatures hydrogen-pressure is reduced to the weight ratio (〉 5wt% of the hydrogen that can satisfy the commercialization requirement) about 700 the atmospheric high pressure of needs.For commercialized running, these technology all do not have competitive power on cost.So people invest hydrogen storage material with attention.USDOE to the business-like target of hydrogen storage material is, the weight ratio of hydrogen in hydrogen storage material is 6.5% under 0～100 degree centigrade (° C) and 1～10 atmospheric condition.Though the various countries scientist is seeking good hydrogen storage material, the development of hydrogen storage material does not at present also relatively slowly break through, and does not have to satisfy the material that USDOE requires.
For solving the problem of fuel cell hydrogen source, people turn to attention and produce the hydrogen material recently.Characteristics of producing the hydrogen material for they can with water direct reaction product hydrogen, thereby in needs for fuel cell provides hydrogen, saved storage and the transportation problem of hydrogen.The present metal hydride that mainly contains as research object is as lithium hydride (LiH), sodium hydride (NaH), magnesium hydride (MgH
2), sodium alanate (NaAlH
4), lithium borohydride (LiBH
4), sodium borohydride (NaBH
4) and POTASSIUM BOROHYDRIDE (KBH
4) etc.Consider various practical factors, be easy to the business-like sodium borohydride (NaBH that has only at present
4).Therefore, as the product hydrogen material of portable use, sodium borohydride (NaBH
4) study at most.Use sodium borohydride (NaBH
4) be to use sodium hydroxide (NaOH) to make solution stabilizer thereby have the highly basic pollution problem as producing the problem that the hydrogen material exists.Simultaneously, use sodium borohydride (NaBH
4) must use catalytic unit and catalyzer to produce hydrogen as producing the hydrogen material, this will increase volume and the cost of system greatly.Another present problem is sodium borohydride (NaBH
4) expensive, be about 55 dollars of per kilograms (US$55/kg), the cost that influence is used.
Producing the another kind of of hydrogen material is metal.Though metallic lithium (Li), sodium (Na) and potassium (K) can be directly with the water reaction and produce hydrogen, the expensive product of reaction simultaneously of these basic metal is that highly basic produces environment and pollutes, so does not have commercial application value.But cheaply and on earth content is abundant for other metal such as iron (Fe) and aluminium prices such as (Al), thereby attractive to people as producing the hydrogen material.Particularly not only atomic mass is light for metallic aluminium (Al), and the electron density height, with the hydrogen amount height of water reaction generation.But at normal temperatures and pressures, metallic iron (Fe) and aluminium (Al) are all very slowly limited with the reaction of water.Metallic aluminium (Al) particularly, its surface can form dense oxide protective membrane of a passivation when being exposed to well-oxygenated environment, and therefore, metallic aluminium (Al) is difficult with the direct reaction of water.
Summary of the invention
The purpose of this invention is to provide a kind of new easy, inexpensive hydrogen manufacturing technique, reach directly complete reaction and produce the purpose of hydrogen of aluminium (Al) and water under certain condition.
The present invention for a kind of be g-Al with the fine aluminium powder at aluminium hydroxide or oxide compound
2O
3, a-Al
2O
3Or TiO
2Produce the processing method of hydrogen under the katalysis with the water reaction, it is characterized in that having following process and step:
A. with the aluminium hydroxide (Al (OH) of a certain amount of micron or nano-scale
3) or oxide compound be g-Al
2O
3, a-Al
2O
3Or TiO
2Powder joins in the closed container that certain water gaging is housed, and the aluminium hydroxide that adds or oxide compound and water are mixed;
B. fine aluminium (Al) powder of a certain amount of micron-scale is directly joined in the above closed container that fills aluminium hydroxide or oxide compound and water mixed solution;
C. namely, make fine aluminium powder and the water successive reaction in the above-mentioned sealed vessel and produce hydrogen namely under 0.04 normal atmosphere at 0.04bar at normal temperatures and pressures or under the normal temperature and vacuum conditions; Its reaction equation is:
Aluminium (Al)+water (3H
2O) → aluminium hydroxide (Al (OH)
3)+hydrogen (3/2H
2↑)
Aluminium hydroxide or oxide compound shared weight percent in whole powder (aluminium powder body+aluminium hydroxide or oxide compound) as catalyzer are 10 wt% to 50 wt%; The temperature of reaction is the normal temperature of 10 ° of C to 40 ° of C, and the environmental stress of reaction is 0.04 atmospheric vacuum to 1 atmospheric normal pressure.
The advantage of the inventive method is as follows:
(1) the present invention need not special and exacting terms, only needs to add in water a certain amount of aluminium hydroxide or oxide compound, and the aluminium powder body just can make hydrogen with the water reaction.
(2) have higher hydrogen output, 1 kilogram aluminium (Al) can produce 0.11 kilogram hydrogen.
(3) just can make hydrogen without any need for soda acid, the by product of reaction is chemically neutral, non-environmental-pollution; And reducible time metal A l of by product of reaction recycles.
(4) the metallic aluminium price is relatively cheap, and the aluminium source is abundant to be obtained easily; The cost that produces 1 kilogram of hydrogen with aluminium (Al) powder is about sodium borohydride (NaBH
4) sixth.
Therefore with aluminium powder system hydrogen portable multikilowatt fuel cell and other small portable fuel cell hydrogen-feedings are had significantly
Price advantage, and have the simple advantage of processing unit.
Description of drawings
Fig. 1 is scanning electronic microscope (SEM) photo of the used powder of the present invention: (a) mean sizes is 7.29 microns original aluminum (Al) powder, and (b) mean sizes is 2.5 microns aluminium hydroxide (Al (OH)
3) powder, (c) specific surface area is 190 m
2The nanometer g-Al of/g
2O
3Powder, (d) specific surface area is 14.46 m
2The nanometer a-Al of/g
2O
3Powder, (e) specific surface area is 27.93 m
2The nano-TiO of/g
2Powder.
Fig. 2 is that fine aluminium (Al) powder is not having catalyzer and using 28 wt% aluminium hydroxides (Al (OH) under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
3) situation under the reaction of metallic aluminium (Al) powder and water produce the progress of hydrogen rate (complete reaction rate) with the reaction times.(illustrate: 28 wt% here refer to aluminium hydroxide shared weight percent in whole powder (aluminium powder body+aluminium hydroxide), and the amount of (aluminium powder body+aluminium hydroxide) is 1 gram in the experiment, and the amount of water is 250 milliliters)
Fig. 3 is that fine aluminium (Al) powder is not having catalyzer and using 34 wt% g-Al under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
2O
3Situation under the reaction of metallic aluminium (Al) powder and water produce the progress of hydrogen rate (complete reaction rate) with the reaction times.(illustrate: 34 wt% here refer to g-Al
2O
3At whole powder (aluminium powder body+g-Al
2O
3) in shared weight percent, (aluminium powder body+g-Al in the experiment
2O
3) amount be 1 the gram, the amount of water is 250 milliliters)
Fig. 4 is that fine aluminium (Al) powder is not having catalyzer and using 39 wt% a-Al under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
2O
3Situation under the reaction of metallic aluminium (Al) powder and water produce the progress of hydrogen rate (complete reaction rate) with the reaction times.(illustrate: 39 wt% here refer to a-Al
2O
3At whole powder (aluminium powder body+a-Al
2O
3) in shared weight percent, (aluminium powder body+a-Al in the experiment
2O
3) amount be 1 the gram, the amount of water is 250 milliliters)
Fig. 5 is that fine aluminium (Al) powder is not having catalyzer and using 40 wt% TiO under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
2Situation under the reaction of metallic aluminium (Al) powder and water produce the progress of hydrogen rate (complete reaction rate) with the reaction times.(illustrate: 40 wt% here refer to TiO
2At whole powder (aluminium powder body+TiO
2) in shared weight percent, (aluminium powder body+TiO in the experiment
2) amount be 1 the gram, the amount of water is 250 milliliters)
Fig. 6 is that fine aluminium (Al) powder is using 34 wt% g-Al under the vacuum condition of normal temperature (25 ° of C) and normal pressure (1bar) or 0.04 normal atmosphere (0.04bar)
2O
3Situation under the reaction of metallic aluminium (Al) powder and water produce the progress of hydrogen rate (complete reaction rate) with the reaction times.(illustrate: 34 wt% here refer to g-Al
2O
3At whole powder (aluminium powder body+g-Al
2O
3) in shared weight percent, (aluminium powder body+g-Al in the experiment
2O
3) amount be 1 the gram, the amount of water is 250 milliliters)
Fig. 7 be under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar) fine aluminium (Al) powder at the g-Al that uses the Different Weight per distribution ratio
2O
3The progress of hydrogen rate (complete reaction rate) with the reaction times produced in the reaction of metallic aluminium (Al) powder and water under the situation of (12 wt%, 34 wt%, 54 wt%).(illustrate: (aluminium powder body+g-Al in the experiment
2O
3) amount be 1 the gram, the amount of water is 250 milliliters).
Fig. 8 is x-ray diffraction pattern, and wherein: a. is at the phase composition of fine aluminium (Al) powder and water reaction after 151 hours under normal temperature (25 ° of C) normal pressure (1bar) condition; B. at the phase composition of fine aluminium (Al) powder and water reaction after 119.3 hours under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar); C. using 34 wt% g-Al under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
2O
3Situation under the phase composition of pure (Al) powder and water reaction after 32.4 hours; D. using 39 wt% a-Al under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
2O
3Situation under the phase composition of pure (Al) powder and water reaction after 38.3 hours; E. using 28 wt% Al (OH) under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
3Situation under the phase composition of pure (Al) powder and water reaction after 29 hours; F. using 40 wt% TiO under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
2Situation under the phase composition of pure (Al) powder and water reaction after 39.8 hours.
Embodiment
After now specific embodiments of the invention being described in.
Embodiment one
The concrete preparation process of present embodiment is as described below:
Get 250 milliliters of (mL) deionized waters and put into the airtight Glass Containers of a known volume, then add the aluminium hydroxide that is used for Catalyzed Aluminum and water reaction, its add-on is 28 wt%, stir with glass stick, add metallic aluminium (Al) powder then, with glass stick all powders and water are stirred again, then that airtight Glass Containers is airtight.With regard to the air pressure in the airtight Glass Containers being evacuated to the vacuum pressure of 0.04 normal atmosphere (0.04bar), begin experiment as the need vacuum then.Because aluminium (Al) only produces hydrogen with the water reaction, therefore we calculate the volume that produces hydrogen by the pressure variation that records in the airtight Glass Containers according to equation for ideal gases, again the total amount that produces hydrogen according to the Al complete reaction that adds calculate metallic aluminium (Al) powder and water the complete reaction rate over time, just produce hydrogen and make progress curve.
At aluminium hydroxide (Al (OH)
3) katalysis under the reaction of Al and water produce the progress of hydrogen referring to Fig. 2; Show under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar), fine aluminium in 45 hours time (Al) will can and not produce hydrogen with the water reaction if powder has aluminium hydroxide to exist, but as the aluminium hydroxide (Al (OH) that adds 28 wt%
3) time, fine aluminium (Al) powder will and produce hydrogen with the water successive reaction after through the inductive phase of one period short period of time (5.5 hours).After through 29 hours, Al and water base complete reaction.
Embodiment two
The preparation process of present embodiment and above-described embodiment 1 are identical, and that different is the g-Al that has adopted 34 wt%
2O
3As catalyzer; At g-Al
2O
3Katalysis under the reaction of Al and water produce the progress of hydrogen referring to Fig. 3; Show that fine aluminium in 45 hours time (Al) is not if powder has g-Al under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
2O
3Existence will can and not produce hydrogen with the water reaction, but as the g-Al that adds 34 wt%
2O
3The time, fine aluminium (Al) powder will and produce hydrogen with the water successive reaction after through the inductive phase of one period short period of time (2.4 hours).After through 32.4 hours, Al and water base complete reaction.
Embodiment three
The preparation process of present embodiment and above-described embodiment 1 are identical, and that different is the a-Al that has adopted 39 wt%
2O
3As catalyzer; At a-Al
2O
3Katalysis under the reaction of Al and water produce the progress of hydrogen referring to Fig. 4; Show that fine aluminium in 45 hours time (Al) is not if powder has a-Al under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
2O
3Existence will can not produce hydrogen with the water reaction, but as the a-Al that adds 39 wt%
2O
3The time, fine aluminium (Al) powder will and produce hydrogen with the water successive reaction after through the inductive phase of one period short period of time (12.1 hours).After through 38.3 hours, Al and water base complete reaction.
Embodiment four
The preparation process of present embodiment and above-described embodiment 1 are identical, and that different is the TiO that has adopted 39 wt%
2As catalyzer; At TiO
2Katalysis under the reaction of Al and water produce the progress of hydrogen referring to Fig. 5; Show that fine aluminium in 45 hours time (Al) is not if powder has TiO under the vacuum condition of normal temperature (25 ° of C) and 0.04 normal atmosphere (0.04bar)
2Existence will can and not produce hydrogen with the water reaction, but as the TiO that adds 40 wt%
2The time, fine aluminium (Al) powder will and produce hydrogen with the water successive reaction after through the inductive phase of one period short period of time (11.2 hours).After through 39.8 hours, Al and water base complete reaction.
About experiment and result and the comment of doing under other condition
(1). under the varying environment air pressure at g-Al
2O
3Katalysis under the reaction of Al and water produce the progress of hydrogen referring to Fig. 6; Show under the vacuum condition of normal temperature (25 ° of C) normal pressure (1bar) or normal temperature and 0.04 normal atmosphere (0.04bar), as long as g-Al is arranged
2O
3Exist, fine aluminium (Al) powder all can and produce hydrogen with the water successive reaction behind inductive phase after a while.Certainly, under vacuum condition, add g-Al
2O
3More obvious with the effect of water reaction product hydrogen to promoting aluminium (Al).
(2). use the g-Al of Different Weight per distribution ratio (12 wt%, 34 wt%, 54 wt%) under the vacuum condition of normal temperature and 0.04 normal atmosphere (0.04bar)
2O
3The complete reaction rate of (Al) powder of metallic aluminium under the situation and water is namely produced the hydrogen progress referring to Fig. 7.Can see that the oxide amount of adding is more many from Fig. 7, more obvious to the effect that promotes aluminium (Al) and water reaction to produce hydrogen.Certainly, when adding g-Al
2O
3Amount when being 54 wt%, g-Al
2O
3Produce the effect of hydrogen as if near saturated to promoting aluminium (Al) and water reaction.
From Fig. 2-5 as can be known, g-Al
2
O
3
And Al (OH)
3
Better to the effect that shortens the reaction inductive phase time and promote aluminium (Al) and water reaction to produce hydrogen.
Fig. 8 shows the reaction hardly at normal temperatures and pressures of metallic aluminium (Al) powder and water, the aluminium hydroxide of adding (Al (OH)
3) or oxide compound (g-Al
2O
3, a-Al
2O
3, TiO
2) phase composition equal no change before and after the reaction of aluminium (Al) powder and water, aluminium hydroxide (Al (OH) is described
3) or oxide compound just the reaction product hydrogen of aluminium (Al) powder and water is played katalysis.The by product that produces hydrogen from the reaction of aluminium (Al) powder and water is bayerite (bayerite (Al (OH)
3)) but the equation of principal reaction be:
Aluminium (Al)+water (3H
2O) → aluminium hydroxide (Al (OH)
3)+hydrogen (3/2H
2↑).
Claims (2)
1. one kind is g-Al with the fine aluminium powder at aluminium hydroxide or oxide compound
2O
3, a-Al
2O
3Or TiO
2Produce the processing method of hydrogen under the katalysis with the water reaction, it is characterized in that having following process and step:
A. with the aluminium hydroxide (Al (OH) of a certain amount of micron or nano-scale
3) or oxide compound be g-Al
2O
3, a-Al
2O
3Or TiO
2Powder joins in the closed container that certain water gaging is housed, and the aluminium hydroxide that adds or oxide compound and water are mixed;
B. fine aluminium (Al) powder of a certain amount of micron-scale is directly joined in the above closed container that fills aluminium hydroxide or oxide compound and water mixed solution;
C. namely, make fine aluminium powder and the water successive reaction in the above-mentioned sealed vessel and produce hydrogen namely under 0.04 normal atmosphere at 0.04bar at normal temperatures and pressures or under the normal temperature and vacuum conditions; Its reaction equation is:
Aluminium (Al)+water (3H
2O) → aluminium hydroxide (Al (OH)
3)+hydrogen (3/2H
2↑).
As claimed in claim 1 under hydrogen aluminium hydroxide or oxide compound katalysis the reaction of aluminium powder body and water produce the processing method of hydrogen, it is characterized in that the aluminium hydroxide as catalyzer is Al (OH)
3, oxide compound is g-Al
2O
3, a-Al
2O
3Or TiO
2, be that shared weight percent is 10 wt% to 50 wt% in (aluminium powder body+aluminium hydroxide or oxide compound) at whole powder; The temperature of reaction is the normal temperature of 10 ° of C to 40 ° of C, and the environmental stress of reaction is 0.04 atmospheric vacuum to 1 atmospheric normal pressure.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103991888A (en) * | 2014-05-26 | 2014-08-20 | 上海大学 | Method for preparing high-activity aluminum hydroxide suspension liquid and producing hydrogen through high-activity aluminum hydroxide suspension liquid and pure aluminum powder reaction |
| CN104291268A (en) * | 2014-05-26 | 2015-01-21 | 上海东科凯乔能源科技有限公司 | Method for preparing hydrogen production material modified aluminum powder through wet chemical technology |
| CN106905112A (en) * | 2017-03-07 | 2017-06-30 | 王亚壮 | A kind of method and system of new synthesizing methanol |
| CN110038571A (en) * | 2019-03-29 | 2019-07-23 | 洛阳师范学院 | The preparation method and application of Fe/AlOOH catalyst |
| CN111410170A (en) * | 2020-04-28 | 2020-07-14 | 江苏汉卓医疗科技有限公司 | Composite material for generating hydrogen and application method and application device thereof |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103991888A (en) * | 2014-05-26 | 2014-08-20 | 上海大学 | Method for preparing high-activity aluminum hydroxide suspension liquid and producing hydrogen through high-activity aluminum hydroxide suspension liquid and pure aluminum powder reaction |
| CN104291268A (en) * | 2014-05-26 | 2015-01-21 | 上海东科凯乔能源科技有限公司 | Method for preparing hydrogen production material modified aluminum powder through wet chemical technology |
| CN103991888B (en) * | 2014-05-26 | 2016-05-25 | 上海大学 | A kind of method of preparing high activity aluminium hydroxide suspension and producing hydrogen with pure aluminium powder precursor reactant |
| CN106905112A (en) * | 2017-03-07 | 2017-06-30 | 王亚壮 | A kind of method and system of new synthesizing methanol |
| CN110038571A (en) * | 2019-03-29 | 2019-07-23 | 洛阳师范学院 | The preparation method and application of Fe/AlOOH catalyst |
| CN110038571B (en) * | 2019-03-29 | 2022-02-08 | 洛阳师范学院 | Preparation method and application of Fe/AlOOH catalyst |
| CN111410170A (en) * | 2020-04-28 | 2020-07-14 | 江苏汉卓医疗科技有限公司 | Composite material for generating hydrogen and application method and application device thereof |
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Application publication date: 20130828 |