CN104513925A - Yttrium-nickel rare earth family hydrogen storage alloy, and secondary battery containing hydrogen storage alloy - Google Patents
Yttrium-nickel rare earth family hydrogen storage alloy, and secondary battery containing hydrogen storage alloy Download PDFInfo
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- CN104513925A CN104513925A CN201410427281.9A CN201410427281A CN104513925A CN 104513925 A CN104513925 A CN 104513925A CN 201410427281 A CN201410427281 A CN 201410427281A CN 104513925 A CN104513925 A CN 104513925A
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- hydrogen storage
- alloy
- storage alloy
- lanthanon
- hydrogen
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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
- Y02E60/10—Energy storage using batteries
Abstract
The invention relates to a yttrium-nickel rare earth family hydrogen storage alloy, and a secondary battery containing the hydrogen storage alloy, and concretely relates to an AB3 type RExYyNiz-a-bMnaAlb hydrogen storage electrode alloy. The alloy has good activation performances, rate discharge ability, and charge and discharge or hydrogen adsorption desorption cycle stability, can be used in a wide temperature range, has small self discharge, and has a highest electrochemical capacity reaching above 360mAh.g<-1>. The alloy has better electrochemical performances and gas phase hydrogen adsorption and desorption performances than traditional LaNi5 type hydrogen storage alloy as a hydrogen storage electrode and a hydrogen storage material respectively, and contains no magnesium element; and the preparation method of the hydrogen storage electrode alloy is simpler and safer than the preparation method of rare earth-magnesium-nickel family AB3 hydrogen storage alloy.
Description
Technical field
The present invention relates to a kind of AB
3type RE-Y-NiMnAl hydrogen storage alloy.
Background technology
Hydrogen storage alloy is that the class found the end of the sixties in last century has the high functional materials storing hydrogen density, and existing hydrogen storage alloy is broadly divided into six classes from composition: Rare Earth AB
5type is as LaNi
5; Magnesium system is as Mg
2ni, MgNi, La
2mg
17; RE-Mg-Ni system AB
3-4type is as La
2mgNi
9, La
5mg
2ni
23, La
3mgNi
14; Titanium system AB type is as TiNi, TiFe; Zirconium, titanium system Laves phase AB
2type is as ZrNi
2; Vanadium system solid solution is as (V
0.9ti
0.1)
1-xfe
x.
Now widely used hydrogen storage material is LaNi
5type hydrogen storage alloy.This alloy is mainly used as the negative material of metal hydride-nickel secondary batteries (MH/Ni), and its theoretical electrochemistry capacity is 373mAhg
-1, the commodity negative material Mm (NiCoMnAl) of practical application
5the about 350mAhg of maximum capacity of (wherein Mm is norium)
-1.In order to develop the hydrogen storage alloy that chemical property is better or hydrogen-storage amount is larger, the research of Magnuminium is given to the attention of height.The theoretical electrochemistry capacity of Mg-base hydrogen-bearing alloy material is high, especially RE-Mg-Ni system AB
3type, A
2b
7type, A
5b
19the research of type hydrogen storage alloy achieves impressive progress, and enters the commercial application stage.Zirconium, titanium system and vanadium system hydrogen storage material are not all widely used owing to activating the too high reason of difficulty, cost.
Document " An electrochemical study of new La
1-xce
xy
2ni
9(0≤x≤1) hydrogen storage alloys " (Electrochimica Acta, 46 (2001): 2385-2393) and document " New ternary intermetallic compoundsbelonging to the R-Y-Ni (R=La, Ce) system as negative electrodes for Ni-MH batteries " (Journalof Alloys and Compounds, 330-332 (2002): 782-786) report AB
3type La-Y-Ni hydrogen storage alloy, but not containing Mn and Al element in alloy, and hydrogen storage capability is the highest only has 260mAhg
-1.
The AB of extensively research at present
3in type RE-Mg-Ni materials base hydrogen storage alloy, Mg element is one of principal constituent.As CN102660700A discloses a kind of AB
3type hydrogen storage alloy and preparation method.AB
3the chemical formula of type hydrogen storage alloy is: La
0.35pr
0.30mg
xni
2.90al
0.30, wherein x=0.30 ~ 0.35.Not containing Y element in this proprietary alloy composition, but must contain Mg element, because the vapour pressure of active metal element magnesium is high, manufacture difficulty be increased, alloying constituent is difficult to control, and the fine magnesium powder simultaneously volatilized is inflammable and explosive and there is potential safety hazard.
Summary of the invention
The present invention aims to provide a kind of lanthanon hydrogen storage alloy not containing Mg element, to overcome deficiency of the prior art.
The present invention relates to a kind of general formula is RE
xy
yni
z-a-bmn
aal
blanthanon hydrogen storage alloy, wherein, one or more elements in RE=La, Ce, Pr, Nd, Sm, Gd, x > 0, y>=0.5, x+y=3; 9.5 > z>=8.5 (are stoichiometric ratio AB during z=9
3type; Be non-stoichiometric AB during z ≠ 9
3type), 3.5>=a+b > 0.
Further, the preferred content range of RE element is 0.5 ~ 2.0;
Further, the preferred content range of Mn element is 0.5 ~ 2.0;
Further, the preferred content range of Al element is 0.2 ~ 1.0.
High melt-quick quenching technique is adopted to prepare alloy, its technological process is as described below: the equal > 99.0% of the purity of each elemental metals or master alloy raw material in composition, calculate according to chemical molecular formula proportioning and accurately take each raw material, raw material is put into Al successively
2o
3crucible, is evacuated to 3.0Pa, is filled with rare gas element Ar to 0.055MPa.Intensification melting, is incubated rapid hardening after about 6min.Rapid hardening copper roller linear velocity is 3.4m/s.Copper roller normal open water coolant, coolant water temperature 25 DEG C.Easy scaling loss raw material need increase proportioning in right amount, increases ratio as following table:
Raw material | RE | Y | Mn | Al |
Increase ratio | 2% | 1% | 5% | 3% |
Except above-mentioned preparation method, RE of the present invention
xy
yni
z-a-bmn
aal
bhydrogen storage alloy can also adopt this area other hydrogen storage alloy preparation method to be prepared, such as: high melt teeming practice, mechanical alloying (MA) method, powder sintering, high melt-gas atomization, reduction-diffusion process, displacement diffusion process, conbustion synthesis (CS) method, self-propagating high-temperature synthesis (SHS) etc.
Present invention also offers a kind of by described RE
xy
yni
z-a-bmn
aal
bthe secondary cell that type hydrogen storage alloy prepares.
RE of the present invention
xy
yni
z-a-bmn
aal
bhydrogen storage alloy also can press different ratios compound with other hydrogen storage material, prepares new hydrogen storage material.
RE of the present invention
xy
yni
z-a-bmn
aal
btype hydrogen storage alloy can adopt heat treating method to improve its weave construction and performance, as: eliminate alloy structure stress and solute segregation, improve hydrogen platform identity or alloy electrode are inhaled/put to alloy charge/discharge platform identity, raising hydrogen-sucking amount and cycle life etc.; Also various surface treatment method can be adopted to improve its performance, as: improve the suction of alloy/put hydrogen or charge/discharge dynamic performance, strengthen the resistance of oxidation of alloy, improve the electrical and thermal conductivity performance etc. of alloy.
AB of the present invention
3type RE
xy
yni
z-a-bmn
aal
bhydrogen storage electrode alloy, have good activation performance, multiplying power discharging ability, discharge and recharge or suction and put hydrogen cyclical stability, can use in wide temperature range, self-discharge is little, and its most high electrochemistry capacitance can reach 360mAhg
-1above.The chemical property of this alloy as hydrogen-storage electrode and the gas phase hydrogen storage property as hydrogen storage material are better than traditional LaNi
5type hydrogen storage alloy, not containing magnesium elements in its composition, with RE-Mg-Ni system AB
3type hydrogen storage alloy is compared, the simple and safety of manufacture method.In addition, in hydrogen storage alloy of the present invention, yttrium (Y) element is one of main component, yttrium aboundresources in the rare earth mineral reserve of China, and the use of this element is conducive to the comprehensive utilization balancing China's rare earth resources.
Accompanying drawing explanation
Fig. 1 is LaY
2ni
8mn
0.5al
0.5the XRD figure of hydrogen storage alloy
Embodiment
Employing preceding method prepares the AB described in embodiment 1 ~ 22
3type RE
xy
yni
z-a-bmn
aal
bhydrogen storage alloy.
Alloy described in embodiment 13 and embodiment 14 adopts identical raw material ratio to obtain.Alloy described in embodiment 13 adopts afore-said hot melting-quick quenching technique preparation, its technological process is: the equal > 99.0% of the purity of each elemental metals or master alloy raw material in composition, calculate according to chemical molecular formula proportioning and accurately take each raw material (easy scaling loss raw material need increase proportioning in right amount), raw material is put into Al successively
2o
3crucible, is evacuated to 3.0Pa, is filled with rare gas element Ar to 0.055MPa.Intensification melting, is incubated rapid hardening after about 6min.Rapid hardening copper roller linear velocity is 3.4m/s.Copper roller normal open water coolant, coolant water temperature 25 DEG C.
Alloy described in embodiment 14 also can adopt high melt-quick quenching technique preparation, annealing heat treatment step is increased in its technological process, be specially: the equal > 99.0% of the purity of each elemental metals or master alloy raw material in composition, calculate according to chemical molecular formula proportioning and accurately take each raw material (easy scaling loss raw material need increase proportioning in right amount), raw material is put into Al successively
2o
3crucible, is evacuated to 3.0Pa, is filled with rare gas element Ar to 0.055MPa.Intensification melting, is incubated rapid hardening after about 6min.Rapid hardening copper roller linear velocity is 3.4m/s.Copper roller normal open water coolant, coolant water temperature 25 DEG C.Rapid hardening alloy slice is under vacuum or protection of inert gas, and anneal at 750 DEG C thermal treatment 8h.
M1 in embodiment 20 is lanthanum rich norium, is wherein about 64% containing La, Ce is about 25%, Pr is about 3%, Nd is about 8%.
The preparation method of test electrode is: embodiment 1 ~ 22 alloy becomes 200-300 object powder through Mechanical Crushing, and alloy powder and carbonyl nickel powder mix with the mass ratio of 1: 4, make under 16MPa pressure
mH electrode slice, this electrode slice is placed between two panels nickel foam, sandwich the nickel strap as lug simultaneously, under 16MPa pressure, again make the storage hydrogen negative pole (MH electrode) for testing, around electrode slice, ensure the close contact between electrode slice and nickel screen by spot welding.
In open type two electrode system of test chemical property, negative pole is MH electrode, and positive pole adopts the sintering Ni (OH) of capacity excess
2/ NiOOH electrode, electrolytic solution is 6molL
-1kOH solution, 24h shelved by the battery assembled, application LAND cell tester measures the chemical property (activation number of times, peak capacity, high-rate discharge capacity HRD, cyclical stability etc.) of alloy electrode with galvanostatic method, and test environment temperature is 298K.Density of charging current 70mAg
-1, duration of charging 6h, discharge current density 70mAg
-1, electric discharge stopping potential is 1.0V, charge and discharge intermittent time 10min.
Following table 1 lists RE described in embodiment 1 ~ 22
xy
yni
z-a-bmn
aal
bhydrogen storage alloy and chemical property thereof.
Table 1 RE
xy
yni
z-a-bmn
aal
bhydrogen storage alloy and chemical property thereof
Note: a is the cycle index that electrode activation needs; B is maximum discharge capacity; C is the capability retention of circulation 100 times; The multiplying power discharging ability that d is discharge current density Id when being 350mAg-1; Discharge capacitance when e is low temperature 243K; F is the capability retention (self-discharge characteristics) after depositing 72 hours.
As seen from Table 1, alloy LaY described in embodiment 13 and 14
2ni
8mn
0.5al
0.5chemical property compare, the electrochemistry capacitance of annealed heat treated embodiment 14 alloy electrode increases, and cycle life, multiplying power discharging ability, cryogenic discharging characteristic, self-discharge performance all make moderate progress.
As shown in Figure 1, x-ray diffractometer is used to analyze LaY
2ni
8mn
0.5al
0.5the weave construction of alloy (embodiment 13), alloy principal phase is YNi
3phase or LaNi
3phase.
Claims (10)
1. a lanthanon hydrogen storage alloy, is characterized in that: composition general formula is RE
xy
yni
z-a-bmn
aal
b, wherein RE is one or more elements in La, Ce, Pr, Nd, Sm, Gd; X > 0, y>=0.5, x+y=3; 9.5 > z>=8.5; 3.5>=a+b > 0.
2. a kind of lanthanon hydrogen storage alloy as claimed in claim 1, is characterized in that: 2.0 >=x >=0.5.
3. a kind of lanthanon hydrogen storage alloy as claimed in claim 1 or 2, is characterized in that: 2.0 >=a >=0.5.
4. a kind of lanthanon hydrogen storage alloy as claimed in claim 1 or 2, is characterized in that: 1.0 >=b >=0.2.
5. a kind of lanthanon hydrogen storage alloy as claimed in claim 1 or 2, is characterized in that: z=9.
6. a kind of lanthanon hydrogen storage alloy as claimed in claim 1, is characterized in that: 2.0 >=x >=0.5,2.0 >=a >=0.5,1.0 >=b >=0.2, z=9.
7. a preparation method for lanthanon hydrogen storage alloy, is characterized in that: calculate according to chemical molecular formula proportioning and accurately take each elemental metals raw material, material purity is all greater than 99.0%; Raw material is put into Al
2o
3crucible, is evacuated to 3.0Pa, is filled with rare gas element Ar to 0.055MPa; Intensification melting, be incubated rapid hardening after about 6min, rapid hardening copper roller linear velocity is 3.4m/s, copper roller normal open water coolant, coolant water temperature 25 DEG C.
8. the preparation method of a kind of lanthanon hydrogen storage alloy as claimed in claim 7, is characterized in that: after rapid hardening step terminates, and alloy is under vacuum or protection of inert gas, and anneal at 750 DEG C thermal treatment 8h.
9. a hydrogen-bearing alloy electrode, is characterized in that using the lanthanon hydrogen storage alloy according to any one of claim 1-6 as hydrogen storage media.
10. a secondary cell, is characterized in that containing hydrogen-bearing alloy electrode according to claim 9.
Priority Applications (5)
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CN201410427281.9A CN104513925B (en) | 2014-08-28 | 2014-08-28 | Yttrium-nickel rare earth family hydrogen storage alloy, and secondary battery containing hydrogen storage alloy |
CN201580046681.8A CN107075617B (en) | 2014-08-28 | 2015-08-27 | A kind of lanthanon hydrogen storage alloy and application thereof |
PCT/CN2015/088274 WO2016029861A1 (en) | 2014-08-28 | 2015-08-27 | Rare-earth based hydrogen storage alloy and application thereof |
JP2017530386A JP6464268B2 (en) | 2014-08-28 | 2015-08-27 | Rare earth hydrogen storage alloy and its use |
US15/507,133 US10566614B2 (en) | 2014-08-28 | 2015-08-27 | Rare earth based hydrogen storage alloy and application thereof |
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CN201410427281.9A CN104513925B (en) | 2014-08-28 | 2014-08-28 | Yttrium-nickel rare earth family hydrogen storage alloy, and secondary battery containing hydrogen storage alloy |
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Cited By (6)
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CN105349865A (en) * | 2015-11-02 | 2016-02-24 | 梅州市星泰环保科技有限公司 | Rare earth alloy |
WO2016029861A1 (en) * | 2014-08-28 | 2016-03-03 | 包头稀土研究院 | Rare-earth based hydrogen storage alloy and application thereof |
CN111471910A (en) * | 2020-04-14 | 2020-07-31 | 包头稀土研究院 | AB3Gadolinium-containing hydrogen storage alloy, electrode, battery and preparation method thereof |
CN114703400A (en) * | 2022-04-24 | 2022-07-05 | 包头稀土研究院 | A5B19Rare earth-yttrium-nickel hydrogen storage alloy, battery and preparation method |
CN114955988A (en) * | 2022-05-30 | 2022-08-30 | 赣州有色冶金研究所有限公司 | Rare earth yttrium-nickel hydrogen storage alloy and preparation method and application thereof |
CN115261675A (en) * | 2022-07-20 | 2022-11-01 | 华南理工大学 | Single-phase or multi-phase AB4La-Y-Ni based superlattice hydrogen storage alloy and preparation method thereof |
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Cited By (10)
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WO2016029861A1 (en) * | 2014-08-28 | 2016-03-03 | 包头稀土研究院 | Rare-earth based hydrogen storage alloy and application thereof |
US10566614B2 (en) | 2014-08-28 | 2020-02-18 | Baotou Research Institute of Rare Earths | Rare earth based hydrogen storage alloy and application thereof |
CN105349865A (en) * | 2015-11-02 | 2016-02-24 | 梅州市星泰环保科技有限公司 | Rare earth alloy |
CN105349865B (en) * | 2015-11-02 | 2017-04-12 | 梅州市星泰环保科技有限公司 | Rare earth alloy |
CN111471910A (en) * | 2020-04-14 | 2020-07-31 | 包头稀土研究院 | AB3Gadolinium-containing hydrogen storage alloy, electrode, battery and preparation method thereof |
CN111471910B (en) * | 2020-04-14 | 2021-12-03 | 包头稀土研究院 | AB3Gadolinium-containing hydrogen storage alloy, electrode, battery and preparation method thereof |
CN114703400A (en) * | 2022-04-24 | 2022-07-05 | 包头稀土研究院 | A5B19Rare earth-yttrium-nickel hydrogen storage alloy, battery and preparation method |
CN114955988A (en) * | 2022-05-30 | 2022-08-30 | 赣州有色冶金研究所有限公司 | Rare earth yttrium-nickel hydrogen storage alloy and preparation method and application thereof |
CN115261675A (en) * | 2022-07-20 | 2022-11-01 | 华南理工大学 | Single-phase or multi-phase AB4La-Y-Ni based superlattice hydrogen storage alloy and preparation method thereof |
CN115261675B (en) * | 2022-07-20 | 2022-12-23 | 华南理工大学 | Single-phase or multi-phase AB 4 La-Y-Ni based superlattice hydrogen storage alloy and preparation method thereof |
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