CN116179898A - Hydrogen-producing aluminum alloy material capable of being rapidly reacted with water and preparation method thereof - Google Patents
Hydrogen-producing aluminum alloy material capable of being rapidly reacted with water and preparation method thereof Download PDFInfo
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- CN116179898A CN116179898A CN202310067955.8A CN202310067955A CN116179898A CN 116179898 A CN116179898 A CN 116179898A CN 202310067955 A CN202310067955 A CN 202310067955A CN 116179898 A CN116179898 A CN 116179898A
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C21/00—Alloys based on aluminium
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- 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
- C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
- C01B3/08—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents with metals
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C1/00—Making non-ferrous alloys
- C22C1/02—Making non-ferrous alloys by melting
- C22C1/026—Alloys based on aluminium
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C21/00—Alloys based on aluminium
- C22C21/06—Alloys based on aluminium with magnesium as the next major constituent
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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 discloses an aluminum alloy material for producing hydrogen by fast reaction with water and a preparation method thereof, wherein the aluminum alloy material comprises the following components in percentage by mass: 0-1% of Mg, 0.8-4% of Ga, 0.5-1% of In, 0.5-1% of Sn, 0.5-1.5% of Bi and the balance of Al. The invention also discloses a preparation method of the aluminum alloy material for preparing hydrogen by fast reaction with water. The aluminum alloy material can produce hydrogen in a neutral aqueous solution medium with a wider temperature range (0-70 ℃), has high hydrogen production rate and high hydrogen production efficiency, and effectively solves the problems of low hydrogen production rate, low hydrogen production efficiency and the like in the prior art under the conditions of low temperature and normal temperature.
Description
Technical Field
The invention relates to the technical field of nonferrous metals, in particular to an aluminum alloy material for producing hydrogen by fast reaction with water and a preparation method thereof.
Background
With the world economic development, the global energy consumption is continuously increased, the extreme climate change generated by the world economic development and the energy consumption is further aggravated, and the development and utilization of novel renewable clean energy are necessary choices for solving the energy crisis, protecting the environment and realizing economic sustainable development. As clean and efficient renewable energy sources, hydrogen energy plays an important role in the development and application of new energy fields, is an ideal energy carrier, is considered as the clean energy source with the most development potential in the twenty-first century, and is researched as strategic energy sources in all countries around the world. Compared with the traditional hydrogen production technology, the aluminum-water reaction hydrogen production technology has the advantages of wide raw material sources, easy control of reaction, low consumption of electric energy, simple system, wide application and the like. Meanwhile, the product of the hydrogen production by the aluminum water reaction can be recycled, and the environmental pollution is small. Therefore, the technology of producing hydrogen by aluminum water reaction is considered as a hydrogen preparation technology with application prospect.
The hydrogen production by the reaction of metal and water is a field hydrogen production mode at normal temperature and normal pressure, and the hydrogen production by the reaction of metal and water comprises the following steps: the advantages of higher mass hydrogen storage density and volume hydrogen storage density, spontaneous operation at normal temperature and pressure, relatively simple hydrogen production device, easy preservation and safety of hydrolysis hydrogen production materials, convenient storage and transportation, basically no toxicity and no harm of reaction byproducts and the like are all paid attention by researchers. The active chemical property and the higher energy density of the metal aluminum are promising energy storage and energy conversion materials, the aluminum is increasingly attracting attention as a novel energy material, and the metal Al is a hydrolysis hydrogen production material which is widely studied. However, the strong oxygen-philic property of aluminum and the formation of a dense oxide film passivation layer on the surface thereof seriously inhibit the continuous reaction with water and have low hydrogen production rate, and a great deal of researches and reports are made on the reaction of activated aluminum and water for hydrogen production. In recent years, the related researches on the aluminum water reaction hydrogen production material at home and abroad mainly comprise: alkaline activation/additive oxide activation, aluminum-carbon composite activation, aluminum salt system activation, aluminum-based alloy activation and the like. Among them, the alloying element is doped into aluminum to obtain aluminum-based alloy for hydrogen production, which is a more effective approach.
The related reports of domestic literature and patents show that the aluminum-based alloy system for producing hydrogen mainly comprises: 1) Aluminum-tin system: al-Sn-X (X: fe, li, snCl) 2 ) Ternary aluminum alloy and aluminum-indium system: al-In-X (X: ga, sn, zn, mgCl) 2 、SnCl 2 ) Ternary aluminum alloys, such as aluminum-tin (Al-Sn) alloys, which were prepared at the earliest reported temperatures of Nagita, etc., react with water at normal temperatures to release hydrogen, but at a slow rate; eom et al, reacted with sodium hydroxide solution at 30 deg.C to produce hydrogen. Hu, yoo et al are prepared by powder metallurgyThe prepared aluminum-tin-carbon nano tube composite material (Al-Sn/CNT) containing 27% of tin has higher hydrogen production rate and hydrogen yield of sodium hydroxide solution at 50 ℃, and the hydrogen production rate of the alloy reaches 6ml/min cm 2 The hydrogen production amount reaches: 700mL/g; 2) The Al-Ga-Sn-In quaternary aluminum alloy is prepared by hydrolysis of an electric arc melting method, such as HE, to prepare a hydrogen Al-3Ga-3In-3Sn alloy block, wherein the maximum hydrogen production rate In pure water at 40 ℃ is 12.3 mL/(min.g) and the maximum hydrogen production amount is 989mL/g, and the maximum hydrogen production rate In pure water at 75 ℃ is 60 mL/min.g and the maximum hydrogen production amount is 1200mL/g; al-Ga-In-Sn alloy prepared by wang of Hubei university of industry reacts with pure water at 60 ℃, the hydrogen yield is higher than 1000ml/g, and the maximum hydrogen yield rate can reach 1080 ml/min.g. Al34Ga-11In-5Sn aluminum alloy prepared by Jeffrey et Al reacts with water at 24 ℃, and the hydrogen production rate reaches 80% In 400 s; 3) Al-Ga-In-Sn-X (X: cu, bi, zn, ti) five-membered aluminum alloy, for example, du Bangdeng, chen Demin of China university of science and technology, researches on the effect of Cu, mg and heat treatment on hydrogen production rate and hydrogen production efficiency of hydrolysis of Al-Ga-In-Sn alloy and the mechanism of aluminum water reaction, wherein the Al-Mg-Ga-In-Sn ageing state alloy with Mg content of 2% is 3 mL/min.g In pure water at 70 ℃, the Al-Mg-Ga-In-Sn ageing state alloy with Cu content of 1% is 150 mL/min.g In pure water at 70 ℃, and the hydrogen production rate is about 45%. The research and analysis of the influence of Zn doping amount on the hydrogen production performance, phase composition and microstructure of the Al-Ga-In-Sn-Zn quinary aluminum alloy prepared by smelting and casting method at Shaanxi university of science and technology and the like and the hydrogen production performance of hydrolysis hydrogen production In water at 40-70 ℃ are carried out, and the analysis of the hydrogen production mechanism is carried out by combining with an aluminum alloy hydrolysate, wherein the Al-Ga-In-Sn-Zn aluminum alloy sample with the Zn content reaching 5 percent has the best hydrogen production performance of hydrolysis hydrogen production In water at 70 ℃ and the maximum average rate of 130mL/min & g of hydrogen production, and the hydrogen production amount: 1020mL/g, and the hydrogen production rate can reach 98 percent; HUANG et Al at Jilin university prepared Al-Ga-In-Sn-Bi five-membered alloy by fusion casting method, the alloy reacts with pure water at normal temperature to generate hydrogen, the maximum hydrogen production rate can reach 15.6 mL/min.g, and the maximum hydrogen production amount can reach 500mL/g. Wang Hongbo, xie Zhixiong, etc. Al-3Ga-3In-3Sn-0.1% AlTi5B alloy block prepared by powder metallurgy method, 1g Al-3Ga-3In-3Sn-0.1% AlTi5B alloy, inReacting with water at 20 ℃ to generate hydrogen with the rate of 3.5 mL/min.g and the hydrogen generation conversion rate of 79.3%;1g Al-5Ga-5Sn-0.5% AlTi5B aluminum alloy reacts with water at 60 ℃ for 20min, the hydrogen production rate is 58.5 mL/min.g, the hydrogen production amount is 1170mL, and the conversion rate is 96%. The related researches on aluminum alloy materials for producing hydrogen by aluminum water reaction are reported to be mostly aqueous solution media with higher temperature (about 60 ℃), and the researches on aluminum alloy materials for producing hydrogen by room-temperature aqueous solution media are reported to be less and the hydrogen production rate is lower. The aluminum alloy material for producing hydrogen by reacting aluminum water at room temperature has less report, so that the aluminum alloy material which has wide application environment and can react at 0-70 ℃ is developed, the online hydrogen production is realized, the instant use is realized, and the practical application value and the application prospect are realized.
Disclosure of Invention
In order to solve the technical problems, the invention aims to provide the aluminum alloy material for producing hydrogen by fast reaction with water and the preparation method thereof, and the aluminum alloy material can produce hydrogen in a neutral aqueous solution medium with a wider temperature range (0-70 ℃), has high hydrogen production rate and high hydrogen production efficiency, and effectively solves the problems of low hydrogen production rate, low hydrogen production efficiency and the like under the conditions of low temperature and normal temperature in the prior art.
The technical scheme for solving the technical problems is as follows: the aluminum alloy material for preparing the hydrogen by fast reaction with water comprises the following components in percentage by mass: 0-1% of Mg, 0.8-4% of Ga, 0.5-1% of In, 0.5-1% of Sn, 0.5-1.5% of Bi and the balance of Al.
Further, the hydrogen production aluminum alloy material by fast reaction with water comprises the following components in percentage by mass: mg0.2%, ga 4%, in 1.5%, sn 1% and Bi 1.5%, the balance being Al.
The preparation method of the hydrogen production aluminum alloy material by the rapid reaction with water comprises the following steps:
(1) Placing Al, mg, ga, in, sn and Bi In a resistance furnace, wherein the smelting temperature is 740-750 ℃, protecting an aluminum alloy solvent, stirring for 10-30min after all melting, and standing for 10-20min to obtain an aluminum alloy casting solution;
(2) Pouring the aluminum alloy casting solution obtained in the step (1) at 720-740 ℃ to obtain the aluminum alloy material for hydrogen production by fast reaction with water.
Further, in step (1), the aluminum alloy solvent is 45% wtNaCl+50% wtKCl+5% wtMgCl 2 。
The invention forms a low-melting point second phase compound and refined grains among alloying elements, utilizes the formation of the low-melting point second phase compound to generate an overburning characteristic, destroys a compact passivation layer structure formed by oxidizing the surface of Al, promotes the continuous reaction of Al and water, thereby generating hydrogen, and simultaneously utilizes the refinement of the grains to generate a large number of grain boundaries, increases the driving force and the number of microcosmic primary cells formed by the grain boundaries and the grains, accelerates the hydrogen evolution reaction of the microcosmic primary cells, ensures more uniform corrosion, generates hydrogen, and improves the hydrogen production rate and the hydrogen production efficiency of the microcosmic primary cells, thereby preparing the hydrogen production aluminum alloy material with high activity, quick reaction with water, high efficiency and safety.
The application of the aluminum alloy material for producing hydrogen by the rapid reaction with water in the hydrogen production of the mobile hydrogen fuel cell.
The invention has the following beneficial effects:
1. the manufacturing process is simple, the operation is convenient, the high-activity aluminum alloy material is safe and environment-friendly, a low-melting-point second-phase compound is formed by adding the anionic low-melting-point alloying element (Ga, in, sn, bi), a compact passivation film structure formed by oxidizing the surface of Al is destroyed, grains are thinned by anodic metal Mg, the driving force of the reaction between grain boundaries and microscopic primary cells of the grains and the number of the microscopic primary cells are increased, the obtained aluminum alloy material (Al-Ga-In-Sn-Bi-Mg) for preparing hydrogen by rapidly reacting with water is corroded more uniformly, and the continuous reaction of Al and water is promoted, so that hydrogen is generated, and the hydrogen production rate and the hydrogen production efficiency are improved; can produce hydrogen at a high rate and high efficiency in a neutral aqueous solution medium with a wider temperature range (0-70 ℃), and effectively solves the problems of low hydrogen production rate, low hydrogen production efficiency and the like in the prior art under the conditions of low temperature and normal temperature.
2. The aluminum alloy material for preparing hydrogen by the rapid reaction with water has high hydrogen production rate in tap water medium at 0-70 ℃, has wide applicable temperature range, and has high hydrogen production rate especially in tap water medium at low temperature (0 ℃); the hydrogen production efficiency is high, and can reach 92-98% in tap water medium at 0-70 ℃.
3. The invention adopts the traditional aluminum alloy smelting and casting method to manufacture, has simple process method and convenient operation; the obtained aluminum alloy material for producing hydrogen by fast reaction with water is a block material, and the storage and the use are safe and convenient; no harmful elements, and the reaction products can be recycled, thus being an environment-friendly material.
Drawings
FIG. 1 is a graph showing the morphology of the product obtained in example 1 before reaction;
FIG. 2 shows the morphology of the product obtained in example 1 after reaction;
FIG. 3 is a morphology of the product obtained in example 2 before reaction;
FIG. 4 shows the morphology of the product obtained in example 2 after reaction.
Detailed Description
The principles and features of the present invention are described below with examples given for the purpose of illustration only and are not intended to limit the scope of the invention. The specific conditions are not noted in the examples and are carried out according to conventional conditions or conditions recommended by the manufacturer. The reagents or apparatus used were conventional products commercially available without the manufacturer's attention.
The hydrogen production rate test method in the examples: the volume of hydrogen produced by the sample in unit mass and unit time in tap water medium with a certain temperature is collected by a drainage method, and the hydrogen production rate is calculated.
Hydrogen production rate = volume of hydrogen (ml)/time (min) sample mass (g);
the method for testing the hydrogen production amount and the hydrogen production efficiency comprises the following steps: and collecting the volume of hydrogen generated by the sample after complete reaction in tap water medium at a certain temperature by using a drainage method, and calculating the hydrogen yield and the hydrogen production efficiency.
Hydrogen production efficiency = volume of hydrogen (ml)/sample mass (g);
1g theoretical hydrogen production volume of Al: 1244ml.
Example 1
The aluminum alloy material for producing hydrogen by fast reaction with water comprises the following components in percentage by mass: ga 4%, in 1.5%, sn 1% and Bi 1.5%, the balance being Al.
The preparation method of the hydrogen production aluminum alloy material by the rapid reaction with water comprises the following steps:
(1) Al, ga, in, sn and Bi are placed In a resistance furnace at 740 ℃ and an aluminum alloy solvent (45% wtNaCl+50% wtKCl+5% wtMgCl) 2 ) Protecting, stirring for 20min after all melting, and standing for 100min to obtain aluminum alloy casting solution;
(2) Casting the aluminum alloy casting solution obtained in the step (1) into round bars with casting phi 30 at the temperature of 730 ℃, and then machining the round bars into cylindrical samples with the diameter of phi 25mm by 20 mm.
The pre-reaction morphology of the cylindrical sample is shown in figure 1, and after the reaction, uneven corrosion pits appear on the surface of the sample, see figure 2; and the hydrogen production rates of the obtained samples in different media are as follows:
medium 1: tap water, temperature: hydrogen production rate at 0 ℃): 920.0 mL/(min.g), hydrogen production amount: 1145mL/g, hydrogen production efficiency: 92.0%.
Medium 2: tap water, temperature: 25 ℃, hydrogen production rate: 1060.0 mL/(min.g), hydrogen production amount: 1160.0mL/g, hydrogen production efficiency: 93.5%.
Medium 3: tap water, temperature: hydrogen production rate at 70 ℃): 1190.0 mL/(min.g), hydrogen production amount: 1180.0mL/g, hydrogen production efficiency: 95.2%.
Example 2
The aluminum alloy material for producing hydrogen by fast reaction with water comprises the following components in percentage by mass: 0.2% of Mg0.2%, 4% of Ga, 1.5% of In, 1% of Sn and 1.5% of Bi, and the balance of Al.
The preparation method of the hydrogen production aluminum alloy material by the rapid reaction with water comprises the following steps:
(1) Al, mg, ga, in, sn and Bi are placed In a resistance furnace, the smelting temperature is 740 ℃, the aluminum alloy solvent is 45 percent wtNaCl+50 percent wtKCl+5 percent wtMgCl 2 ) Protecting, stirring for 20min after all melting, and standing for 100min to obtain aluminum alloy casting solution;
(2) Casting the aluminum alloy casting solution obtained in the step (1) into round bars with casting phi 30 at the temperature of 730 ℃, and then machining the round bars into cylindrical samples with the diameter of phi 25mm by 20 mm.
FIG. 3 is a graph showing the morphology of a cylinder sample with added alloying element Mg before reaction; after the reaction, the surface of the sample added with the alloy element Mg is corroded uniformly, as shown in FIG. 4, and the hydrogen production rate of the obtained sample in different media is as follows:
medium 1: tap water, temperature: hydrogen production rate at 0 ℃): 910.0 mL/(min.g), hydrogen production amount: 1146mL/g, hydrogen production efficiency: 92.0%.
Medium 2: tap water, temperature: 25 ℃, hydrogen production rate: 1040.0 mL/(min.g), hydrogen production amount: 1159.0mL/g, hydrogen production efficiency: 93.5%.
Medium 3: tap water, temperature: hydrogen production rate at 70 ℃): 1190.0 mL/(min.g), hydrogen production amount: 1181.0mL/g, hydrogen production efficiency: 95.2%.
Example 3
The aluminum alloy material for producing hydrogen by fast reaction with water comprises the following components in percentage by mass: 0.2% of Mg0.2%, 2% of Ga, 0.8% of In, 0.5% of Sn and 0.8% of Bi, and the balance of Al.
The preparation method of the hydrogen production aluminum alloy material by the rapid reaction with water comprises the following steps:
(1) Al, mg, ga, in, sn and Bi are placed In a resistance furnace, the smelting temperature is 740 ℃, the aluminum alloy solvent is 45 percent wtNaCl+50 percent wtKCl+5 percent wtMgCl 2 ) Protecting, stirring for 20min after all melting, and standing for 100min to obtain aluminum alloy casting solution;
(2) Casting the aluminum alloy casting solution obtained in the step (1) into round bars with casting phi 30 at the temperature of 730 ℃, and then machining the round bars into cylindrical samples with the diameter of phi 25mm by 20 mm.
The hydrogen production rates of the obtained samples in different media are as follows:
medium 1: tap water, temperature: hydrogen production rate at 0 ℃): 820.60 mL/(min.g), hydrogen production amount: 1152mL/g, hydrogen production efficiency: 92.7%.
Medium 2: tap water, temperature: 25 ℃, hydrogen production rate: 960.0 mL/(min.g), hydrogen production amount: 1177.0mL/g, hydrogen production efficiency: 94.6%.
Medium 3: tap water, temperature: hydrogen production rate at 70 ℃): 1170.0 mL/(min.g), hydrogen production amount: 1192.0mL/g, hydrogen production efficiency: 96%.
Example 4
The aluminum alloy material for producing hydrogen by fast reaction with water comprises the following components in percentage by mass: 0.2% of Mg0.2%, 1% of Ga, 0.8% of In, 0.5% of Sn and 0.8% of Bi, and the balance of Al.
The preparation method of the hydrogen production aluminum alloy material by the rapid reaction with water comprises the following steps:
(1) Al, mg, ga, in, sn and Bi are placed In a resistance furnace, the smelting temperature is 740 ℃, the aluminum alloy solvent is 45 percent wtNaCl+50 percent wtKCl+5 percent wtMgCl 2 ) Protecting, stirring for 20min after all melting, and standing for 100min to obtain aluminum alloy casting solution;
(2) Casting the aluminum alloy casting solution obtained in the step (1) into round bars with casting phi 30 at the temperature of 730 ℃, and then machining the round bars into cylindrical samples with the diameter of phi 25mm by 20 mm.
The hydrogen production rates of the obtained samples in different media are as follows:
medium 1: tap water, temperature: hydrogen production rate at 0 ℃): 620.0 mL/(min.g), hydrogen production amount: 1170mL/g, hydrogen production efficiency: 94.4%.
Medium 2: tap water, temperature: 25 ℃, hydrogen production rate: 900.0 mL/(min.g), hydrogen production amount: 1185.0mL/g, hydrogen production efficiency: 95.6%.
Medium 3: tap water, temperature: hydrogen production rate at 70 ℃): 1120.0 mL/(min.g), hydrogen production amount: 1200.0mL/g, hydrogen production efficiency: 98.0%.
The foregoing description of the preferred embodiments of the invention is not intended to limit the invention to the precise form disclosed, and any such modifications, equivalents, and alternatives falling within the spirit and scope of the invention are intended to be included within the scope of the invention.
Claims (5)
1. The aluminum alloy material for producing hydrogen by fast reaction with water is characterized by comprising the following components in percentage by mass: 0-1% of Mg, 0.8-4% of Ga, 0.5-1% of In, 0.5-1% of Sn, 0.5-1.5% of Bi and the balance of Al.
2. The rapid reaction with water hydrogen production aluminum alloy material as claimed in claim 1, comprising the following components in percentage by mass: mg0.2%, ga 4%, in 1.5%, sn 1% and Bi 1.5%, the balance being Al.
3. The method for preparing the hydrogen-producing aluminum alloy material by rapid reaction with water as claimed in claim 1 or 2, characterized by comprising the steps of:
(1) Placing Al, mg, ga, in, sn and Bi In a resistance furnace, wherein the smelting temperature is 740-750 ℃, protecting an aluminum alloy solvent, stirring for 10-30min after all melting, and standing for 10-20min to obtain an aluminum alloy casting solution;
(2) Pouring the aluminum alloy casting solution obtained in the step (1) at 720-740 ℃ to obtain the aluminum alloy material for hydrogen production by fast reaction with water.
4. A method for producing a hydrogen producing aluminum alloy material by rapid reaction with water as claimed in claim 3, wherein in step (1), said aluminum alloy solvent is 45% wtnacl+50% wtkcl+5% wtmgcl 2 。
5. Use of the aluminum alloy material for producing hydrogen by rapid reaction with water according to claim 1 or 2 in hydrogen production of mobile hydrogen fuel cells.
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2023
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