CN106001543A - Method for modifying La-Mg-Ni based hydrogen storage alloy by utilizing Ni-B-C alloy - Google Patents
Method for modifying La-Mg-Ni based hydrogen storage alloy by utilizing Ni-B-C alloy Download PDFInfo
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- CN106001543A CN106001543A CN201610401758.5A CN201610401758A CN106001543A CN 106001543 A CN106001543 A CN 106001543A CN 201610401758 A CN201610401758 A CN 201610401758A CN 106001543 A CN106001543 A CN 106001543A
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- 229910045601 alloy Inorganic materials 0.000 title claims abstract description 34
- 239000000956 alloy Substances 0.000 title claims abstract description 34
- 229910001339 C alloy Inorganic materials 0.000 title claims abstract description 28
- 229910020791 La—Mg—Ni Inorganic materials 0.000 title claims abstract description 28
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 20
- 239000001257 hydrogen Substances 0.000 title claims abstract description 20
- 238000000034 method Methods 0.000 title claims abstract description 16
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title abstract description 8
- 238000000498 ball milling Methods 0.000 claims abstract description 31
- 239000000843 powder Substances 0.000 claims abstract description 29
- 239000000463 material Substances 0.000 claims abstract description 9
- 238000000227 grinding Methods 0.000 claims abstract description 6
- 239000001996 bearing alloy Substances 0.000 claims description 12
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims description 12
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 10
- 229910000521 B alloy Inorganic materials 0.000 claims description 10
- 239000000203 mixture Substances 0.000 claims description 10
- 238000012986 modification Methods 0.000 claims description 7
- 230000004048 modification Effects 0.000 claims description 7
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 5
- 238000013019 agitation Methods 0.000 claims description 5
- 229910052786 argon Inorganic materials 0.000 claims description 5
- 239000012153 distilled water Substances 0.000 claims description 5
- 230000006698 induction Effects 0.000 claims description 5
- 238000002844 melting Methods 0.000 claims description 5
- 230000008018 melting Effects 0.000 claims description 5
- 239000002184 metal Substances 0.000 claims description 5
- 238000005406 washing Methods 0.000 claims description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 5
- 230000014759 maintenance of location Effects 0.000 abstract description 4
- 238000011161 development Methods 0.000 abstract description 2
- 229910052987 metal hydride Inorganic materials 0.000 abstract 1
- 229910018095 Ni-MH Inorganic materials 0.000 description 4
- 229910018477 Ni—MH Inorganic materials 0.000 description 4
- 239000000126 substance Substances 0.000 description 3
- 230000004087 circulation Effects 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 229910000808 amorphous metal alloy Inorganic materials 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F1/00—Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
- B22F1/14—Treatment of metallic powder
-
- B22F1/0003—
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F9/00—Making metallic powder or suspensions thereof
- B22F9/02—Making metallic powder or suspensions thereof using physical processes
- B22F9/04—Making metallic powder or suspensions thereof using physical processes starting from solid material, e.g. by crushing, grinding or milling
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C19/00—Alloys based on nickel or cobalt
- C22C19/03—Alloys based on nickel or cobalt based on nickel
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/24—Alkaline accumulators
- H01M10/30—Nickel accumulators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/383—Hydrogen absorbing alloys
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F9/00—Making metallic powder or suspensions thereof
- B22F9/02—Making metallic powder or suspensions thereof using physical processes
- B22F9/04—Making metallic powder or suspensions thereof using physical processes starting from solid material, e.g. by crushing, grinding or milling
- B22F2009/041—Making metallic powder or suspensions thereof using physical processes starting from solid material, e.g. by crushing, grinding or milling by mechanical alloying, e.g. blending, milling
-
- 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
- Y02E60/10—Energy storage using batteries
Abstract
The invention discloses a method for modifying a La-Mg-Ni based hydrogen storage alloy by utilizing a Ni-B-C alloy. The method comprises the following steps: preparing the La-Mg-Ni based hydrogen storage alloy and Ni-B-C alloy powder respectively, and then uniformly mixing the La-Mg-Ni based hydrogen storage alloy and the Ni-B-C alloy powder according to a mass ratio; and after the uniform mixing, carrying out ball milling, wherein the ratio of the mixed material in a ball mill to a grinding medium is 20:1, the rotating speed of the ball mill is 150-200 rpm, and the ball milling period is 0.5-1.0 h. Accordingly, the La-Mg-Ni based hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20 can be modified by utilizing the Ni-B-C alloy. The method disclosed by the invention is simple to operate; after the Ni-B-C alloy powder is added, both the maximum discharge capacity and the capacity retention ratio of an electrode can be improved; and the method has certain practical significance to the development of nickel-metal hydride batteries.
Description
Technical field
The invention belongs to materials chemistry and electrochemical research field, particularly to a kind of Ni-B-C alloy utilizing ball milling to obtain to La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20The method being modified.
Background technology
Along with the enhancing of people's environmental consciousness, hybrid vehicle will have broader market.In the existing hybrid-power battery market share, 98% is Ni-MH power cell.The negative material of Ni-MH battery is mainly hydrogen bearing alloy, and La-Mg-Ni base hydrogenous alloy has than business-like AB5The unit cell volume that type lanthanon hydrogen storage alloy is bigger, can accommodate more hydrogen and have bigger discharge capacity.La-Mg-Ni base hydrogenous alloy fails to substitute AB5The main cause of type hydrogen storage alloy is that cyclical stability is poor, and this is the difficulty being badly in need of now overcoming.
Research worker is noticed, Co-X (X=B, S, P, Si etc.) amorphous alloy has good chemical property.Researcher, by Co powder and P powder ball milling, makes the negative pole of Ni/MH battery, investigates its chemical property, finds that maximum discharge capacity reaches 300 mAh/g, and after 100 circulations, capability retention is 95%.
The alloy powder of the Ni-B-C that ball-milling method is obtained by the present invention and La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Ball milling after mixing, is all improved as the negative pole of Ni/MH battery, maximum discharge capacity and cyclical stability in varing proportions.
Summary of the invention
It is an object of the invention to provide one utilizes Ni-B-C alloy to La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20The method being modified.
Thinking of the present invention: use ball milling to obtain Ni-B-C alloy, more by a certain percentage with La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Ball milling obtains composite alloy, to improve its chemical property so that it is the negative material as Ni-MH battery is more preferably applied.
Concretely comprise the following steps:
(1) according to hydrogen bearing alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh purity raw metal more than 99%, under argon shield, prepare hydrogen bearing alloy by vacuum induction melting method, will grind after ingot overturning remelting 2 ~ 3 times, cross 200 mesh sieves, prepare La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) in 500 mL distilled water, 15 g NiCl are added2·6H2O, under 95 DEG C of magnetic agitation, the NaBH of dropping 100 ~ 200 mL 0.1 mol/L4Solution, products therefrom absolute ethanol washing 2 times, under the conditions of 75 DEG C, it is dried 5 h obtains Ni-B alloy powder, it is that 6:4 mix homogeneously with graphite powder according to mass ratio by Ni-B alloy powder, rotating speed ball milling 5 ~ 10 h with 200 ~ 400 rpm, ball milling, than for 10:1 or 20:1, i.e. prepares Ni-B-C alloy powder.
(3) the La-Mg-Ni base hydrogenous alloy La that step (1) is prepared0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20The Ni-B-C alloy powder prepared with step (2) is according to ball milling after mass ratio mix homogeneously, ratio of grinding media to material is 20:1, drum's speed of rotation is 150 ~ 200 rpm, Ball-milling Time 0.5 ~ 1.0 h, i.e. realizes utilizing Ni-B-C alloy modification La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
Described mass ratio is 9:1,8.5:1.5 or 8:2.
The Ni-B-C alloy powder that ball milling is obtained by the inventive method by ball milling adds hydrogen bearing alloy La to0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20In, simple to operate, and after interpolation Ni-B-C alloy powder, maximum discharge capacity and the capability retention of electrode are all improved, and the development to Ni-MH battery has certain realistic meaning.
Detailed description of the invention
Embodiment
1
:
(1) according to hydrogen bearing alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh the raw metal that purity is 99.9%, under argon shield, prepare hydrogen bearing alloy by vacuum induction melting method, will grind after ingot overturning remelting 3 times, cross 200 mesh sieves, prepare La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) in 500 mL distilled water, 15 g NiCl are added2·6H2O, under 95 DEG C of magnetic agitation, drips the NaBH of 100 mL 0.1 mol/L4Solution, products therefrom absolute ethanol washing 2 times, under the conditions of 75 DEG C, it is dried 5 h obtains Ni-B alloy powder, it is that 6:4 mix homogeneously with graphite powder according to mass ratio by Ni-B alloy powder, with rotating speed ball milling 10 h of 200 rpm, ball milling, than for 10:1, i.e. prepares Ni-B-C alloy powder.
(3) the La-Mg-Ni base hydrogenous alloy La that step (1) is prepared0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20The Ni-B-C alloy powder prepared with step (2) is 20:1 according to ball milling after mass ratio 9:1 mix homogeneously, ratio of grinding media to material, and drum's speed of rotation is 150 rpm, Ball-milling Time 1.0 h, i.e. realizes utilizing Ni-B-C alloy modification La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
Embodiment
2
:
(1) according to hydrogen bearing alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh the raw metal that purity is 99.9%, under argon shield, prepare hydrogen bearing alloy by vacuum induction melting method, will grind after ingot overturning remelting 3 times, cross 200 mesh sieves, prepare La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) in 500 mL distilled water, 15 g NiCl are added2·6H2O, under 95 DEG C of magnetic agitation, drips the NaBH of 200 mL 0.1 mol/L4Solution, products therefrom absolute ethanol washing 2 times, under the conditions of 75 DEG C, it is dried 5 h obtains Ni-B alloy powder, it is that 6:4 mix homogeneously with graphite powder according to mass ratio by Ni-B alloy powder, with rotating speed ball milling 5 h of 400 rpm, ball milling, than for 20:1, i.e. prepares Ni-B-C alloy powder.
(3) the La-Mg-Ni base hydrogenous alloy La that step (1) is prepared0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20The Ni-B-C alloy powder prepared with step (2) is according to ball milling after mass ratio 8.5:1.5 mix homogeneously, ratio of grinding media to material is 20:1, drum's speed of rotation is 200 rpm, Ball-milling Time 0.5 h, i.e. realizes utilizing Ni-B-C alloy modification La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
Embodiment
3
:
(1) according to hydrogen bearing alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh the raw metal that purity is 99.9%, under argon shield, prepare hydrogen bearing alloy by vacuum induction melting method, will grind after ingot overturning remelting 2 times, cross 200 mesh sieves, prepare La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) in 500 mL distilled water, 15 g NiCl are added2·6H2O, under 95 DEG C of magnetic agitation, drips the NaBH of 150 mL 0.1 mol/L4Solution, products therefrom absolute ethanol washing 2 times, under the conditions of 75 DEG C, it is dried 5 h obtains Ni-B alloy powder, it is that 6:4 mix homogeneously with graphite powder according to mass ratio by Ni-B alloy powder, with rotating speed ball milling 7.5 h of 300 rpm, ball milling, than for 20:1, i.e. prepares Ni-B-C alloy powder.
(3) the La-Mg-Ni base hydrogenous alloy La that step (1) is prepared0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20The Ni-B-C alloy powder prepared with step (2) is 20:1 according to ball milling after mass ratio 8:2 mix homogeneously, ratio of grinding media to material, and drum's speed of rotation is 200 rpm, Ball-milling Time 0.5 h, i.e. realizes utilizing Ni-B-C alloy modification La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
Measure cyclical stability and the dynamic performance of above-described embodiment modified alloy respectively with LAND 5.3B battery test system and CHI 660E electrochemical workstation, result is as follows:
(1) maximum discharge capacity of unmodified alloy electrode is 346 mAh/g, after itself and Ni-B-C alloy powder are according to the ratio ball-milling of 9:1,8.5:1.5,8:2, the electrode maximum discharge capacity obtained is respectively increased 363 mAh/g, 366 mAh/g and 360 mAh/g.
The 70% of the capability retention never modified electrode of (2) 50 circulation rear electrodes increases to 77%, 75% and 77%.
Claims (1)
1. the method utilizing Ni-B-C alloy modification La-Mg-Ni base hydrogenous alloy, it is characterised in that concretely comprise the following steps:
(1) according to hydrogen bearing alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh purity raw metal more than 99%, under argon shield, prepare hydrogen bearing alloy by vacuum induction melting method, will grind after ingot overturning remelting 2 ~ 3 times, cross 200 mesh sieves, prepare La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20;
(2) in 500 mL distilled water, 15 g NiCl are added2·6H2O, under 95 DEG C of magnetic agitation, drips 100 ~ 200
The NaBH of mL 0.1 mol/L4Solution, products therefrom absolute ethanol washing 2 times, under the conditions of 75 DEG C, it is dried 5 h obtains Ni-B alloy powder, it is that 6:4 mix homogeneously with graphite powder according to mass ratio by Ni-B alloy powder, rotating speed ball milling 5 ~ 10 h with 200 ~ 400 rpm, ball milling, than for 10:1 or 20:1, i.e. prepares Ni-B-C alloy powder;
(3) the La-Mg-Ni base hydrogenous alloy La that step (1) is prepared0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20The Ni-B-C alloy powder prepared with step (2) is according to ball milling after mass ratio mix homogeneously, and ratio of grinding media to material is 20:1, and drum's speed of rotation is 150 ~ 200
Rpm, Ball-milling Time 0.5 ~ 1.0 h, i.e. realize utilizing Ni-B-C alloy modification La-Mg-Ni base hydrogenous alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20;
Described mass ratio is 9:1,8.5:1.5 or 8:2.
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN108493436A (en) * | 2018-03-09 | 2018-09-04 | 燕山大学 | Ni-based quaternary hydrogen-storing alloy electrode material of a kind of super stacking provisions lanthanum-M-magnesium-of 2H types A5B19 and preparation method thereof |
CN110492086A (en) * | 2019-09-09 | 2019-11-22 | 燕山大学 | A kind of preparation method of hydrogen storing alloy composite material |
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Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
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CN108493436A (en) * | 2018-03-09 | 2018-09-04 | 燕山大学 | Ni-based quaternary hydrogen-storing alloy electrode material of a kind of super stacking provisions lanthanum-M-magnesium-of 2H types A5B19 and preparation method thereof |
CN110492086A (en) * | 2019-09-09 | 2019-11-22 | 燕山大学 | A kind of preparation method of hydrogen storing alloy composite material |
CN110492086B (en) * | 2019-09-09 | 2021-01-26 | 燕山大学 | Preparation method of hydrogen storage alloy composite material |
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