CN105958024A - Method for improving electrochemical performance of AB3-type hydrogen storage alloy by using Co-B-C alloy - Google Patents

Method for improving electrochemical performance of AB3-type hydrogen storage alloy by using Co-B-C alloy Download PDF

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CN105958024A
CN105958024A CN201610401766.XA CN201610401766A CN105958024A CN 105958024 A CN105958024 A CN 105958024A CN 201610401766 A CN201610401766 A CN 201610401766A CN 105958024 A CN105958024 A CN 105958024A
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hydrogen storage
type hydrogen
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黄红霞
谢文强
于文婉
王新颖
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Guilin University of Technology
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    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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    • 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
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    • H—ELECTRICITY
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    • Y02E60/10—Energy storage using batteries

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Abstract

The invention discloses a method for improving electrochemical performance of AB3-type hydrogen storage alloy by using Co-B-C alloy. The method comprises the following steps: respectively preparing the AB3-type hydrogen storage alloy and Co-B-C alloy powder, and then carrying out ball-milling after uniformly mixing the two components proportionally, wherein the ball material ratio is 20: 1, the rotate speed of a ball mill is 150-200 rpm, and the ball-milling time is 0.5-1.0 h, namely the improvement for the electrochemical performance of La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20 by using the Co-B-C alloy is completed; and the mass proportion is 8: 2, 7: 3, 6: 4, 5: 5 or 4: 6. The method disclosed by the invention is simple in operation, and after the Co-B-C alloy powder is added, the maximum discharge capacity and capacity retention ratio of the electrode are both improved, so that certain practical significance is achieved for the development of nickel-metal hydride batteries.

Description

Co-B-C alloy is utilized to improve AB3The method of type hydrogen storage alloy chemical property
Technical field
The invention belongs to materials chemistry, metallurgical chemistry and electrochemical research field, utilize Co-B-C particularly to one Alloy improves AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20The method of chemical property.
Background technology
Between the many decades in past, traditional AB5Type hydrogen storage alloy is widely used in the negative material of MH/Ni secondary cell. Along with the development of society, its relatively low discharge capacity cannot meet the demand of people.New A B3Type hydrogen storage alloy is considered as more Having the negative material of the MH/Ni battery of development prospect, maximum discharge capacity, up to 410 mAh/g, compares AB5Type alloy is high by 30%, But AB3The easy efflorescence of type alloy, cyclical stability are poor, also fail to commercialization.Researcher uses multiple method to improve AB3Type hydrogen storage is closed Gold cycle performance, such as fluorination treatment, Method of element substitution, chemical plating etc..
In recent years, a series of cobalt and nonmetallic amorphous alloy granule were (such as Co-B, Co-P, Co-S, Co-Si, Co- BH etc.), nanocrystalline metal be used as hydrogen storage material, they all show bigger discharge capacity.Researcher is by Co-S alloy Powder ball milling 20 h, makes the negative pole of MH/Ni battery, and when discharge current density is 25 mA/g, maximum discharge capacity is 350 MAh/g, the discharge capacity after 100 circulations is 300 mAh/g, and capability retention is 86%.The present invention passes through ball-milling method by Co- B-C alloy adds alloy La in varing proportions to0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20In, to improve its cyclical stability And chemical property.
Summary of the invention
It is an object of the invention to provide one utilizes Co-B-C alloy to improve AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20The method of chemical property.
Concretely comprise the following steps:
(1) according to AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh purity 99% Above raw metal, under argon shield, prepares alloy by vacuum induction melting method, after ingot overturning remelting 2 ~ 3 times, and will The ingot casting of remelting grinds, and crosses 200 mesh sieves, prepares AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) under magnetic agitation, toward the CoCl of 200～300 mL 0.1 mol/L2Solution drips 0.1 mol/L's NaBH4Solution 50 ~ 100 mL, products therefrom washes of absolute alcohol 2 ~ 3 times, it is subsequently placed in 5 h in 343 K baking ovens, obtains Co- B alloy powder, by Co-B alloy powder and graphite powder with 6:4 mass than mixing homogeneously after, with rotating speed in planetary ball mill 200 ~ 400 rpm ball milling 5 ~ 10 h, ratio of grinding media to material is 20:1 or 10:1, i.e. prepares Co-B-C alloy powder.
(3) AB prepared by step (1)3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20With step (2) The Co-B-C alloy powder of preparation is according to ball milling after mass ratio mix homogeneously, and ratio of grinding media to material is 20:1, drum's speed of rotation 150 ~ 200 Rpm, Ball-milling Time 0.5 ~ 1.0 h, i.e. complete to utilize Co-B-C alloy to improve AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Chemical property.
Described mass ratio is 8:2,7:3,6:4,5:5 or 4:6.
Co-B-C alloy powder is joined AB by ball-milling method by the inventive method3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20In, simple to operate, and after interpolation Co-B-C alloy powder, the maximum electric discharge of electrode Capacity and capability retention are all improved, and this has certain realistic meaning to the development of Ni-MH battery.
Detailed description of the invention
Embodiment 1:
(1) according to AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh purity and exist The raw metal of 99.9%, under argon shield, prepares alloy by vacuum induction melting method, after ingot overturning remelting 2 times, and will The ingot casting of remelting grinds, and crosses 200 mesh sieves, prepares AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) under magnetic agitation, toward the CoCl of 300 mL 0.1 mol/L2Solution drips the NaBH of 0.1 mol/L4Molten Liquid 100 mL, products therefrom washes of absolute alcohol 3 times, it is subsequently placed in 5 h in 343 K baking ovens, obtains Co-B alloy powder, will Co-B alloy powder and graphite powder with 6:4 mass than mixing homogeneously after, with rotating speed 200 rpm ball milling 10 in planetary ball mill H, ratio of grinding media to material is 20:1, i.e. prepares Co-B-C alloy powder.
(3) AB prepared by step (1)3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20With step (2) The Co-B-C alloy powder of preparation is 20:1 according to ball milling after mass ratio 8:2 mix homogeneously, ratio of grinding media to material, drum's speed of rotation 150rpm, Ball-milling Time 1.0 h, i.e. complete to utilize Co-B-C alloy to improve AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Chemical property.
Embodiment 2:
(1) according to AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh purity and exist The raw metal of 99.9%, under argon shield, prepares alloy by vacuum induction melting method, after ingot overturning remelting 3 times, and will The ingot casting of remelting grinds, and crosses 200 mesh sieves, prepares AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) under magnetic agitation, toward the CoCl of 200 mL 0.1 mol/L2Solution drips the NaBH of 0.1 mol/L4Molten Liquid 50 mL, products therefrom washes of absolute alcohol 3 times, it is subsequently placed in 5 h in 343 K baking ovens, obtains Co-B alloy powder, will Co-B alloy powder and graphite powder with 6:4 mass than mixing homogeneously after, with rotating speed 400 rpm ball milling 5 in planetary ball mill H, ratio of grinding media to material is 10:1, i.e. prepares Co-B-C alloy powder.
(3) AB prepared by step (1)3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20With step (2) The Co-B-C alloy powder of preparation is 20:1 according to ball milling after mass ratio 7:3 mix homogeneously, ratio of grinding media to material, drum's speed of rotation 200 Rpm, Ball-milling Time 0.5 h, i.e. complete to utilize Co-B-C alloy to improve AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Chemical property.
Embodiment 3:
(1) according to AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh purity and exist The raw metal of 99.9%, under argon shield, prepares alloy by vacuum induction melting method, after ingot overturning remelting 2 times, and will The ingot casting of remelting grinds, and crosses 200 mesh sieves, prepares AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) under magnetic agitation, toward the CoCl of 300 mL 0.1 mol/L2Solution drips the NaBH of 0.1 mol/L4Molten Liquid 100 mL, products therefrom washes of absolute alcohol 3 times, it is subsequently placed in 5 h in 343 K baking ovens, obtains Co-B alloy powder, will Co-B alloy powder and graphite powder with 6:4 mass than mixing homogeneously after, with rotating speed 300 rpm ball milling in planetary ball mill 7.5h, ratio of grinding media to material is 20:1, i.e. prepares Co-B-C alloy powder.
(3) AB prepared by step (1)3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20With step (2) The Co-B-C alloy powder of preparation is 20:1 according to ball milling after mass ratio 6:4 mix homogeneously, ratio of grinding media to material, drum's speed of rotation 200 Rpm, Ball-milling Time 0.5 h, i.e. complete to utilize Co-B-C alloy to improve AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Chemical property.
Embodiment 4:
(1) according to AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh purity and exist The raw metal of 99.9%, under argon shield, prepares alloy by vacuum induction melting method, after ingot overturning remelting 3 times, and will The ingot casting of remelting grinds, and crosses 200 mesh sieves, prepares AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) under magnetic agitation, toward the CoCl of 250 mL 0.1 mol/L2Solution drips the NaBH of 0.1 mol/L4Molten Liquid 75 mL, products therefrom washes of absolute alcohol 3 times, it is subsequently placed in 5 h in 343 K baking ovens, obtains Co-B alloy powder, will Co-B alloy powder and graphite powder with 6:4 mass than mixing homogeneously after, with rotating speed 400 rpm ball milling 5 in planetary ball mill H, ratio of grinding media to material is 10:1, i.e. prepares Co-B-C alloy powder.
(3) AB prepared by step (1)3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20With step (2) The Co-B-C alloy powder of preparation is 20:1 according to ball milling after mass ratio 5:5 mix homogeneously, ratio of grinding media to material, drum's speed of rotation 150 Rpm, Ball-milling Time 1.0 h, i.e. complete to utilize Co-B-C alloy to improve AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Chemical property.
Embodiment 5:
(1) according to AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh purity and exist The raw metal of 99.9%, under argon shield, prepares alloy by vacuum induction melting method, after ingot overturning remelting 2 times, and will The ingot casting of remelting grinds, and crosses 200 mesh sieves, prepares AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20。
(2) under magnetic agitation, toward the CoCl of 200 mL 0.1 mol/L2Solution drips the NaBH of 0.1 mol/L4Molten Liquid 50 mL, products therefrom washes of absolute alcohol 2 times, it is subsequently placed in 5 h in 343 K baking ovens, obtains Co-B alloy powder, will Co-B alloy powder and graphite powder with 6:4 mass than mixing homogeneously after, with rotating speed 200 rpm ball milling 10 in planetary ball mill H, ratio of grinding media to material is 20:1, i.e. prepares Co-B-C alloy powder.
(3) AB prepared by step (1)3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20With step (2) The Co-B-C alloy powder of preparation is 20:1 according to ball milling after mass ratio 4:6 mix homogeneously, ratio of grinding media to material, drum's speed of rotation 200 Rpm, Ball-milling Time 0.5 h, i.e. complete to utilize Co-B-C alloy to improve AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Chemical property.
Measure above-described embodiment modification with LAND 5.3B battery test system and CHI 660E electrochemical workstation to close The cyclical stability of the made electrode of gold and dynamic performance, result is as follows:
1) maximum discharge capacity of unmodified electrode is 346 mAh/g, with Co-B-C powder with 8:2,7:3,6:4,5:5,4:6 The electrode maximum discharge capacity that ball-milling obtains be respectively 345 mAh/g, 355 mAh/g, 381 mAh/g, 386 mAh/g and 393 mAh/g。
2) the 70% of the capability retention never modified alloy electrode of 50 circulation rear electrodes increases to successively
80%, 82%, 83%, 73% and 72%.It is attached to AB3Co-B-C alloyed powder on type hydrogen storage alloy surface enhances alloy Resistance to corrosion.
From above-mentioned test result it can be seen that the present invention effectively improves AB3The discharge capacity of type hydrogen storage alloy and circulation Stability.

Claims (1)

1. one kind utilizes Co-B-C alloy to improve AB3The method of type hydrogen storage alloy chemical property, it is characterised in that concrete steps For:
(1) according to AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Mol ratio weigh purity 99% with On raw metal, under argon shield, prepare alloy by vacuum induction melting method, after ingot overturning remelting 2 ~ 3 times, will weight Molten ingot casting grinds, and crosses 200 mesh sieves, prepares AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20；
(2) under magnetic agitation, toward the CoCl of 200～300 mL 0.1 mol/L2Solution drips the NaBH of 0.1 mol/L4Molten Liquid 50 ~ 100 mL, products therefrom washes of absolute alcohol 2 ~ 3 times, it is subsequently placed in 5 h in 343 K baking ovens, obtains Co-B alloyed powder End, by Co-B alloy powder and graphite powder with 6:4 mass than mixing homogeneously after, with rotating speed 200 ~ 400 in planetary ball mill Rpm ball milling 5 ~ 10 h, ratio of grinding media to material is 20:1 or 10:1, i.e. prepares Co-B-C alloy powder；
(3) AB prepared by step (1)3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Prepare with step (2) Co-B-C alloy powder according to ball milling after mass ratio mix homogeneously, ratio of grinding media to material is 20:1, drum's speed of rotation 150 ~ 200 Rpm, Ball-milling Time 0.5 ~ 1.0 h, i.e. complete to utilize Co-B-C alloy to improve AB3Type hydrogen storage alloy La0.94Mg0.06Ni3.49Co0.73Mn0.12Al0.20Chemical property；
Described mass ratio is 8:2,7:3,6:4,5:5 or 4:6.
CN201610401766.XA 2016-06-09 2016-06-09 Method for improving electrochemical performance of AB3-type hydrogen storage alloy by using Co-B-C alloy Pending CN105958024A (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108247040A (en) * 2018-01-10 2018-07-06 内蒙古科技大学 Nano-oxide catalyst coats the in-situ synthesis of hydrogen storing alloy composite material
CN110241350A (en) * 2019-06-03 2019-09-17 中盈志合吉林科技股份有限公司 Cupric cobalt boron hydrogen storage material and its preparation method and application

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CN1794496A (en) * 2005-10-27 2006-06-28 天津大学 Hydrogen storage alloy powder surface cladded with nickel boron alloy and its preparation method
CN104846224A (en) * 2015-05-17 2015-08-19 桂林理工大学 Method for performing surface modification on AB3-type hydrogen storage alloy by utilization of graphene

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CN104846224A (en) * 2015-05-17 2015-08-19 桂林理工大学 Method for performing surface modification on AB3-type hydrogen storage alloy by utilization of graphene

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108247040A (en) * 2018-01-10 2018-07-06 内蒙古科技大学 Nano-oxide catalyst coats the in-situ synthesis of hydrogen storing alloy composite material
CN108247040B (en) * 2018-01-10 2019-08-20 内蒙古科技大学 Nano-oxide catalyst coats hydrogen storing alloy composite material and preparation method thereof
CN110241350A (en) * 2019-06-03 2019-09-17 中盈志合吉林科技股份有限公司 Cupric cobalt boron hydrogen storage material and its preparation method and application

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Application publication date: 20160921