CN1095423A - Hydrogen-storing alloy electrode material - Google Patents
Hydrogen-storing alloy electrode material Download PDFInfo
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- CN1095423A CN1095423A CN94112039A CN94112039A CN1095423A CN 1095423 A CN1095423 A CN 1095423A CN 94112039 A CN94112039 A CN 94112039A CN 94112039 A CN94112039 A CN 94112039A CN 1095423 A CN1095423 A CN 1095423A
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- Prior art keywords
- alloy
- hydrogen
- rich
- electrode material
- lanthanum
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- 229910045601 alloy Inorganic materials 0.000 title claims abstract description 59
- 239000000956 alloy Substances 0.000 title claims abstract description 59
- 239000007772 electrode material Substances 0.000 title claims abstract description 17
- 239000000126 substance Substances 0.000 claims abstract description 8
- 229910052746 lanthanum Inorganic materials 0.000 abstract description 15
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 abstract description 12
- 229910000636 Ce alloy Inorganic materials 0.000 abstract description 6
- 229910000858 La alloy Inorganic materials 0.000 abstract description 6
- 230000004913 activation Effects 0.000 abstract description 5
- 239000000463 material Substances 0.000 abstract description 2
- 238000003860 storage Methods 0.000 description 18
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 16
- 230000005518 electrochemistry Effects 0.000 description 9
- 239000007858 starting material Substances 0.000 description 9
- 239000010936 titanium Substances 0.000 description 9
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 8
- 229910018007 MmNi Inorganic materials 0.000 description 8
- 239000001257 hydrogen Substances 0.000 description 8
- 229910052739 hydrogen Inorganic materials 0.000 description 8
- 238000005275 alloying Methods 0.000 description 7
- 229910001122 Mischmetal Inorganic materials 0.000 description 6
- 229910052759 nickel Inorganic materials 0.000 description 6
- 229910052684 Cerium Inorganic materials 0.000 description 5
- 150000004678 hydrides Chemical class 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 description 4
- 230000004087 circulation Effects 0.000 description 4
- 239000000843 powder Substances 0.000 description 4
- 229910052779 Neodymium Inorganic materials 0.000 description 3
- 229910052777 Praseodymium Inorganic materials 0.000 description 3
- 239000010949 copper Substances 0.000 description 3
- -1 hydride-nickel Chemical compound 0.000 description 3
- 230000006698 induction Effects 0.000 description 3
- 238000011068 loading method Methods 0.000 description 3
- 230000014759 maintenance of location Effects 0.000 description 3
- 229910052748 manganese Inorganic materials 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 2
- 229910001069 Ti alloy Inorganic materials 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 230000006866 deterioration Effects 0.000 description 2
- 238000003411 electrode reaction Methods 0.000 description 2
- 239000008151 electrolyte solution Substances 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 238000002844 melting Methods 0.000 description 2
- 230000008018 melting Effects 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 229910000480 nickel oxide Inorganic materials 0.000 description 2
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 229910052761 rare earth metal Inorganic materials 0.000 description 2
- 150000002910 rare earth metals Chemical class 0.000 description 2
- 238000007789 sealing Methods 0.000 description 2
- 229910000714 At alloy Inorganic materials 0.000 description 1
- 229910000952 Be alloy Inorganic materials 0.000 description 1
- 229910018657 Mn—Al Inorganic materials 0.000 description 1
- 239000004677 Nylon Substances 0.000 description 1
- YZCKVEUIGOORGS-IGMARMGPSA-N Protium Chemical compound [1H] YZCKVEUIGOORGS-IGMARMGPSA-N 0.000 description 1
- 241000720974 Protium Species 0.000 description 1
- 229910001093 Zr alloy Inorganic materials 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 239000012670 alkaline solution Substances 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 239000003963 antioxidant agent Substances 0.000 description 1
- 230000003078 antioxidant effect Effects 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 229910052790 beryllium Inorganic materials 0.000 description 1
- 229910002056 binary alloy Inorganic materials 0.000 description 1
- 238000005266 casting Methods 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 230000002950 deficient Effects 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- 238000007598 dipping method Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000007772 electroless plating Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 239000006260 foam Substances 0.000 description 1
- 238000013467 fragmentation Methods 0.000 description 1
- 238000006062 fragmentation reaction Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 150000002603 lanthanum Chemical class 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000007773 negative electrode material Substances 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 229920001778 nylon Polymers 0.000 description 1
- 238000012856 packing Methods 0.000 description 1
- 235000011837 pasties Nutrition 0.000 description 1
- 150000004965 peroxy acids Chemical class 0.000 description 1
- 238000007747 plating Methods 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
Classifications
-
- 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
Landscapes
- Battery Electrode And Active Subsutance (AREA)
Abstract
A kind of hydrogen-storing alloy electrode material is characterized in that chemical formula is M1Ni
5-x-y-zCo
xMn
yTi
z, M1 is a lanthanum rich norium in the formula, x=0.5～1.0, and y=0.3～0.6, z=0.03～0.1, the chemical formula of preferentially selecting for use is M1Ni
3.45Co
1.0Mn
0.5Ti
0.05And M1Ni
3.75Co
0.8Mn
0.4Ti
0.05Use the battery that material of the present invention is made, item technical performance indexs such as its activation performance, initial capacity, high-rate discharge ability, cycle life all are better than the battery that existing rich lanthanum alloy and rich cerium alloy are made.
Description
The present invention relates to a kind of with the electrode of alloy synthetics as active material, particularly lanthanum rich rare earth hydrogen-storing alloy electrode material.
People utilize the electrochemical properties of hydrogen-storage alloy reversible hydrogen adsorption and desorption, the hydrogen-storage alloy hydride-nickel secondary battery of making, because specific energy height, non-environmental-pollution and noticeable, hydrogen-storage alloy as hydride-nickel-based battery negative electrode active material material should satisfy following basic demand: (1) has higher electrochemistry capacitance and suitable equilibrium hydrogen pressure (10 in battery operated temperature-20 ℃～60 ℃ scope
-4～0.1MPa); (2) energy antioxidant anticorrosive in high alkali liquid has long cycle life; (3) easily-activated, the reversibility of electro catalytic activity and electrode reaction is good; (4) cheap.Its main type of hydrogen-storage alloy that has developed around these basic demands has: AB
5Type is as LaNi
5Be alloy and mishmetal-nickel system alloy; AB
2The titanium alloy of type and zirconium alloy; AB/A
2Type B titanium alloy etc.AB wherein
5Mishmetal-the nickel system hydrogen storage alloy of type because functional, cost is lower, becomes in small-sized sealing hydride-nickel-based battery suitability for industrialized production first-selected hydrogen-storing alloy electrode material.
Different according to La in the norium starting material with the Ce content ratio, form lanthanum rich mischmetal hydrogen-storage alloy and cerium-rich mischmetal hydrogen-storage alloy two big series.Studies show that, because ree content such as La, Ce, Pr, Nd and ratio have significant effects to the performance of hydrogen-storage alloy in the norium, therefore must be at norium starting material dissimilar, the different places of production, adopt different Alloying Treatment modes, just might develop the hydrogen-storing alloy electrode material that satisfies above-mentioned high performance requirements.About the cerium-rich mischmetal hydrogen-storing alloy electrode material, great deal of experimental has been carried out in PANASONIC, Sanyo, the subordinate's of Toshiba Battery Company and the test of Osaka industrial technology, all adopts alloying elements such as Co, Al, Mn partly to substitute MmNi
5In Ni, wherein representative hydrogen-storing alloy electrode material is:
The MmNi that European patent EP-271043 provides
3.55Mn
0.4Al
0.3Co
0.75;
The MmNi that Japanese Patent JP63-264869 provides
3.8Al
0.3Mn
0.4Co
0.5;
J.Less-Common Met., 174, P1195, the MmNi of 1991 reports
3.5Al
0.8Co
0.7And MmNi
3.5Al
0.3Mn
0.4Co
0.8;
The 180th Meeting of the Electrochmical Society, Proceedings Vol 9.2-5 P92, the Mm(Ni-Co-Mn-Al of 1992 reports)
x, x=4.5～4.8.
The defective of above-mentioned cerium-rich mischmetal hydrogen-storing alloy electrode material is: the difficult activation of (1) hydrogen-occlussion alloy electrode, and must be before the preparation electrode through peracid, alkaline solution dipping or Electroless Plating Ni surface modification treatment such as (or Cu); (2) its electrochemistry capacitance is not high enough, and not surface treated alloy only reaches 199～235mAh/g(Japanization association will, No.11, P.1294,1992); (3) because Al generates fine and close oxide film at alloy surface the electrode reaction resistance is increased, cause high-multiplying power discharge and low temperature performance deterioration etc.
About the research of lanthanum rich mischmetal hydrogen-storing alloy electrode material, report is very few so far.Japanese battery company and electrical machinery of Japanese sanyo company adopt the starting material of lanthanum content up to the lanthanum rich mixed rare earth metal Lm of 75～90wt%, at this starting material middle-weight rare earths Elements C e, Pr, Nd, each content all is lower than 10%, be used to make hydrogen-storing alloy electrode material, the disclosed hydrogen-storage alloy composition of the JP03-274239 of Japanese battery house journal is LmNi
X-A-BCo
AAl
B, as LmNi
3.8Co
0.7Al
0.5; The hydrogen-storage alloy Lm of JP03-274240 company of electrical machinery of Japanese sanyo house journal
1-xZr
xNi
Y-A-BCo
AAl
B, as Lm
0.95Zr
0.05Ni
4.0Co
0.5Al
0.5Above-mentioned rich lanthanum alloy and rich cerium alloy MmNi
3.5Co
0.7Al
0.8Relatively, its initial capacity and high-rate discharge ability increase, and behind the electroless copper 20%, initial capacity can reach 268～286mAh/g in advance, high-rate discharge ability C(300mA)/C(20mA) value is 59～77%.And the initial capacity of rich cerium alloy is 254mAh/g, its C(300mA)/C(20mA) be 43%.But the cycle life of above-mentioned rich lanthanum alloy is relatively poor, and after 300 circulations, the capability retention of electrode is 71～89%, follows the target of practicability to also have very big distance.
The objective of the invention is to utilize a kind of resourceful lanthanum rich norium as starting material, a kind of excellent combination property is provided, meet the lanthanum rich mischmetal series hydrogen storage alloy electrode materials that practicability requires.
The objective of the invention is characteristics, by meticulous multi-element alloyed the realization according to homemade lanthanum rich norium raw material resources.
The lanthanum rich norium Ml that the present invention selects for use, its trade mark are RELa-40, and the starting material middle-weight rare earths total metal content of this trade mark is not less than 98wt%, La content 44～51wt% wherein, Ce content 3～5wt%, Pr content 9～11wt%, Nd content 27～41wt%.Ml is starting material with this lanthanum rich norium, and the chemical formula of making hydrogen-storing alloy electrode material is
M1 is that the trade mark is the norium of RELa-40 in the formula, x=0.5～1.0, y=0.3～0.6, z=0.03～0.1.The chemical formula of preferentially selecting for use is:
With prior art relatively, the present invention has following outstanding advantage:
1. selected starting material and nickel are founded the alloy MlNi that forms
5, decapacitation keeps LaNi
5Outside the easy activation that is had, little, the plateau pressure of lagging behind are easy to regulate, aspect effectively hydrogen storage amount and dynamic performance, be better than LaNi
5With rich cerium alloy MmNi
5Three kinds of AB
5The hydride that the type binary alloy is inhaled behind the hydrogen is respectively: MlNi
5H
7, LaNi
5H
6, MmNi
5H
6.5Because the plateau pressure of rich lanthanum alloy hydride is that 0.38MPa is more much lower than rich cerium alloy hydride in the time of 20 ℃, therefore the present invention need not to add Al and the plateau pressure of alloy hydride can be adjusted to easily the practical requirement that meets battery in implementing alloying process.And prior art need be added volume Al and certainly will be caused electrochemistry capacitance to reduce and the high-rate discharge ability deterioration.
2. the present invention has taken into full account the influence of various alloying elements to over-all propertieies such as the plateau pressure of alloy hydride electrode, electrochemistry capacitance, high-multiplying power discharge, cycle lives, and mutual restricting relation, adopt Co, Mn, three kinds of alloying elements of Ti to substitute MlNi
5In part Ni, and the best by meticulous each alloying element of adjusting substitutes amount and proportioning, thereby obtains the Ml(Ni-Co-Mn-Ti of excellent combination property)
5The type hydrogen-storing alloy electrode material.
3. the present invention selects for use Ti as alloying element, and its advantage is: (1) Ti inhales protium, substitutes the electrochemistry capacitance that Ni can further improve hydrogen-storage alloy in right amount; (2) trace Ti can significantly improve the resistance to corrosion of alloy at the oxide film that alloy surface forms in working cycle, and suppresses the oxidized and electrode capacity decline that causes of La.Prior art is added Zr, consequently when improving alloy electrode cycle life, causes electrochemistry capacitance to reduce.
4. use the battery that hydrogen-storing alloy electrode material of the present invention is made, item technical indicators such as its activation performance, initial capacity, high-rate discharge ability, cycle life all significantly are better than prior art.
Embodiment 1:
Make hydrogen-storage alloy MlNi
3.45Co
1.0Mn
0.5Ti
0.05, it is the RELa-40 norium that Ml adopts the trade mark, Ni, Co, Mn, Ti purity are 99%; above-mentioned starting material are weighed by the chemical formula proportioning; drying is placed in the alumina crucible of vacuum induction furnace, and induction furnace is through the exhaust of finding time, melting and pour into ingot casting under the argon gas atmosphere protection.The pressure-resistant reaction vessel of packing into after the alloy fragmentation that obtains, put the hydrogen circulation through the gaseous state suction and be ground into 300～400 purpose powder, powdered alloy and 500 purpose electrolytic copper powders is even by 1: 4 mixed, and being pressed into diameter is that 10mm, thickness are the disk shape hydrogen-occlussion alloy electrode of 0.68mm.In the opening electrolyzer, with the hydrogen-occlussion alloy electrode is negative pole, nickel oxide electrode is anodal, the Hg/HgO electrode is a reference electrode, the 6MKOH aqueous solution is as electrolytic solution, with the constant current charge of 30mA/g alloy 16 hours, respectively with 50mA/g and two kinds of different discharge-rates discharges of 800mA/g alloy, measure the electrochemistry capacitance C of hydrogen-storage alloy then
1And C
2, with C
1Characterize the initial capacity of alloy, (1-C
2/ C
1) the alloy electrochemistry capacitance descended when % was illustrated in high-multiplying power discharge percentage ratio.The cycle life of hydrogen-storage alloy is with the constant current discharge of 100mA/g alloy, and test is through the conservation rate (%) of alloy electrochemistry capacitance after 300 times and 500 charge and discharge cycles, and the stopping potential of above discharge process is-600mV.
Test result shows, above-mentioned not surface treated rich lanthanum MlNi
3.45CO
1.0Mn
0.5Ti
0.05The initial capacity of alloy is 305mAh/g, is higher than existing rich cerium alloy (199-254mAh/g) and rich lanthanum copper-beryllium (268-286mAh/g).The C of reflection high-rate discharge ability
2/ C
1Index is 83.83%, also is better than existing rich cerium and rich lanthanum alloy.The capability retention of alloy is 92.34% after 300 charge and discharge cycles, obviously be better than existing rich lanthanum alloy (71-89%), the capability retention of above-mentioned alloy of the present invention after 500 circulations still can reach 89.6%, illustrates that this alloy has good comprehensive performances.
Embodiment 2:
Melting obtains consisting of MlNi in vacuum induction furnace
3.75Co
0.8Mn
0.4Ti
0.05Hydrogen-storage alloy, alloy is put the hydrogen circulation through the gaseous state suction and is ground into 300～400 order powder, behind chemical nickel plating with alloy powder with 2%PVA solution furnishing pasty state and be filled in the nickel foam sheet, becoming thickness through the roll extrusion attenuate is 0.4mm, dry back is as the hydrogen-storage alloy negative pole, with the nickel oxide electrode is anodal, nylon nonwoven fabrics is a barrier film, with 6MKOH+LiOH is electrolytic solution, be assembled into AA type sealing Ni/MH test cell, only need 1～3 activation can reach the loading capacity index of standard-required behind this battery seal, the loading capacity that records battery when different discharge-rate is:
Discharge-rate 0.2C 1C 2C 3C 5C
Loading capacity (mAh/g) 1,210 1,050 986 950 906
Above-mentioned battery is pressed the IEC standard testing cycle operation life-span, cycle life＞500 weeks.
Claims (2)
1, a kind of hydrogen-storing alloy electrode material contains the norium element, it is characterized in that: its chemical formula is:
Ml is that the trade mark is the norium of RELa-40 in the formula, x=0.5～1.0, y=0.3～0.6, z=0.03～0.1.
2, according to the hydrogen-storing alloy electrode material of claim 1, it is characterized in that: preferentially select for use chemical formula to be:
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN94112039A CN1095423A (en) | 1994-01-31 | 1994-01-31 | Hydrogen-storing alloy electrode material |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN94112039A CN1095423A (en) | 1994-01-31 | 1994-01-31 | Hydrogen-storing alloy electrode material |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN1095423A true CN1095423A (en) | 1994-11-23 |
Family
ID=5035851
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN94112039A Pending CN1095423A (en) | 1994-01-31 | 1994-01-31 | Hydrogen-storing alloy electrode material |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN1095423A (en) |
-
1994
- 1994-01-31 CN CN94112039A patent/CN1095423A/en active Pending
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