CN1738084A - AB5 type negative pole hydrogen-storage material - Google Patents
AB5 type negative pole hydrogen-storage material Download PDFInfo
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- CN1738084A CN1738084A CNA2005100999026A CN200510099902A CN1738084A CN 1738084 A CN1738084 A CN 1738084A CN A2005100999026 A CNA2005100999026 A CN A2005100999026A CN 200510099902 A CN200510099902 A CN 200510099902A CN 1738084 A CN1738084 A CN 1738084A
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- 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
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- Y02E60/10—Energy storage using batteries
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Abstract
The invention provides a AB5 type negative hydrogen storage material. Wherein, the atom proportion is MmNi3.55-xGaxCo0.75Mn0.4Al0.3, in which the x ranges from 0-0.3, the Mm is rare-earth compound formed by La, Ce, Pr and Nd elements, the weight of rare-earth compound Mm is selected as standard, the weight of La is 64.5-67.5 %, the weight of Ce is 22.0-24.0 %, the weight of Pr is 2.5-3.5 % and the weight of Nd is 7.0-9.0 %. Since the Ga is imported, the electrochemical capacity of AB5 type negative hydrogen storage material in low temperature is improved markedly while it can be used in wide range of temperature. So the AB5 type negative hydrogen storage material can be used as negative electrode material to prepare nickel-hydrogen battery with better charging and discharging property in low temperature.
Description
Technical field
The present invention relates to AB
5Type battery cathode hydrogen storage material.Especially, the present invention relates to be used to satisfy the AB of the Ni-MH battery that cryogenic property requires
5The type cathode hydrogen storage material.
Background technology
Because wireless chargeable electric tool fast development brings great convenience to people's work, therefore the battery requirements amount to rechargeable also increases greatly in recent years.The rechargeable battery that is used for electric tool in the past mainly is a nickel-cadmium cell, but the nickel-cadmium cell capacity is lower, has serious environmental again and pollutes, and belongs to obsolete product.Ni-MH battery is with its high power capacity, long-life, excellent specific property such as pollution-free, and similar with the voltage of nickel-cadmium cell, thereby becomes best substitute.Because using the purpose of electric tool is for convenience, therefore there is very big mobility its field of employment, possible temperature can be very low in some special places, this has just proposed requirement to battery discharge performance at low temperatures, and Ni-MH battery product of the prior art, the capacity of battery makes electric tool to use along with the reduction of temperature can occur descending comparatively fast even the phenomenon of can not putting electricity.Ni-MH battery mainly is made up of nickel hydroxide positive plate, hydrogen storage alloy negative, barrier film, potassium hydroxide electrolyte.The performance of entire cell and the performance of each parts are all closely bound up, the capacity that the main cause that the capacity of battery descends along with the temperature reduction is a negative material reduces with temperature and descends comparatively fast, therefore be badly in need of cathode hydrogen storage material with better cryogenic property, the hydrogen storage material that research and development have good low temperature charge discharge characteristic just becomes very urgent.
For Ni-MH battery, used negative material mainly is mishmetal MmNi at present
5-type hydrogen storage alloy, alloy capacity are generally about 300mAh, and in order to improve the capacity of negative pole hydrogen bearing alloy, that is developing at present has a Zr-base AB
2Type Laves' phases alloy, Ti-Zr base AB type alloy and A
2Type B Mg
2The Ni magnesium base alloy, but remove small part AB owing to activating reasons such as slow or cycle life difference
2Outside the type alloy, other alloys all do not reach practical application.
Therefore, for satisfying the needs that cryogenic property had the Ni-MH battery product of requirement, the applicant is with present widely used MmNi
5-type hydrogen storage alloy is a research object, by adding different element kinds therein, thereby has proposed a kind of cathode hydrogen storage material that has the high electrochemical charge/discharge capacity at low temperatures.
Summary of the invention
The objective of the invention is to obtain a kind of (40～30 ℃) at low temperatures than the much higher cathode hydrogen storage material of present commercially available prod charge discharge capacity, to satisfy the Ni-MH battery product that cryogenic property is had requirement by the composition improvement.
Specifically, the invention provides a kind of AB that is applicable to Ni-MH battery
5The type cathode hydrogen storage material, it has the good low temperature charge-discharge performance, this AB
5The atomic ratio composition of type cathode hydrogen storage material consists of MmNi
3.55-xGa
xCo
0.75Mn
0.4Al
0.3, 0＜x≤0.3 wherein, Mm is the lucium of being made up of La, Ce, Pr, Nd element, and the weight with lucium Mm is benchmark, and the content of La is 64.5-67.5wt%, and the content of Ce is 22.0-24.0wt%, the content of Pr is 2.5-3.5wt%, and the content of Nd is 7.0-9.0wt%.
AB
5Hydrogen bearing alloy be by the elements A of easy generation stable hydride (as Mm, Ca, Zr) intermetallic compound of forming with other element B (as Ni, Al, Mn, Si, Zn, Cr, Fe, Cu, Co etc.) belongs to CaCu
5The type hexagonal structure, its charge discharge capacity is mainly derived to inhale and puts in the hydrogen process, come from hydrogen ion in the electrolyte electron transfer in the oxidation-reduction process takes place on hydrogen-bearing alloy electrode, known ni-MH battery electrochemical cell reacts with following discharging and recharging usually to be represented:
Charging
At negative pole, when applying an electrode potential to negative electrode, the hydrogen atom that water decomposed in the electrolyte is inhaled in the alloy, and hydroxide ion is left in the electrolyte:
At positive pole, the charging reaction is the oxidation of hickelous nydroxide (identical with nickel-cadmium cell):
Discharge:
At negative pole, hydrogen is released and is combined into water with hydroxide ion, contributes an electronics simultaneously and forms electric current.
At positive pole, nickel hydroxide is reduced into the lower valency hickelous nydroxide.
The hydrogen bearing alloy that uses for nickel-hydrogen battery at present mainly is made up of Mm, Ni, Co, Mn, Al, and typical composition is MmNi
3.55Co
0.75Mn
0.4Al
0.3, wherein Mm is a mishmetal, and main component is La, Ce, Pr, Nd, and this alloy descends very fast with temperature reduction electrochemistry capacitance as seen from Figure 1.In the present invention, by adding discovering of different alloying elements, in alloy, add element gallium replacement nickel the low temperature charge-discharge performance of alloy is obviously improved, thereby obtain a kind of cathode hydrogen storage material that satisfies the instructions for use of low temperature nickel hydrogen battery.Therefore, based on above result of study, the present invention proposes a kind of low temperature AB that uses for nickel-hydrogen battery
5Type cathode hydrogen storage material, the one-tenth of this material are grouped into (atomic ratio) and are: MmNi
3.55-xGa
xCo
0.75Mn
0.4Al
0.3(0＜x≤0.3), wherein the composition of mishmetal Mm is formed as shown in table 1.
Each constituent content in table 1 mishmetal
| Element | Percentage by weight (wt%) |
| La | 64.5-67.5 |
| Ce | 22.0-24.0 |
| Pr | 2.5-3.5 |
| Nd | 7.0-9.0 |
Preferably, AB of the present invention
5In the type cathode hydrogen storage material, 0.15≤x≤0.3.
As AB of the present invention
5The example of type cathode hydrogen storage material, atomic ratio one-tenth is grouped into and can be:
MmNi
3.50Ga
0.05Co
0.75Mn
0.4Al
0.3；
MmNi
3.45Ga
0.10Co
0.75Mn
0.4Al
0.3；
MmNi
3.40Ga
0.15Co
0.75Mn
0.4Al
0.3；
MmNi
3.35Ga
0.20Co
0.75Mn
0.4Al
0.3；
MmNi
3.30Ga
0.25Co
0.75Mn
0.4Al
0.3Or
MmNi
3.25Ga
0.30Co
0.75Mn
0.4Al
0.3, or the like.
Wherein, most preferred AB
5The type cathode hydrogen storage material is MmNi
3.30Ga
0.25Co
0.75Mn
0.4Al
0.3
AB of the present invention
5The type cathode hydrogen storage material can adopt conventional smelting method for preparing.
For example; can be Mm: Ni: Ga: Co: Mn: Al=1: (3.55-x): x with mol ratio: 0.75: 0.4: 0.3 raw material be inserted the vaccum sensitive stove that vacuumizes the back and feed argon shield and is carried out melting and be cast into ingot casting; 0＜x≤0.3 wherein; Mm is the lucium of being made up of La, Ce, Pr, Nd element; and the weight with lucium Mm is benchmark; the content of La is 64.5-67.5%; the content of Ce is 22.0-24.0%; the content of Pr is 2.5-3.5%, and the content of Nd is 7.0-9.0%.
AB of the present invention
5The type cathode hydrogen storage material can be used for preparing the negative pole of Ni-MH battery.Adopt AB of the present invention
5The type cathode hydrogen storage material has good low temperature charge-discharge performance as the Ni-MH battery of negative pole.
With the AB that sells in the market
5The type hydrogen storage material is (as the traditional cathode hydrogen storage material MmNi for preparing with identical smelting technology
3.55Co
0.75Mn
0.4Al
0.3) compare AB of the present invention
5Type cathode hydrogen storage material MmNi
3.55-xGa
xCo
0.75Mn
0.4Al
0.3(0＜x≤0.3) has improved electrochemistry capacitance at low temperatures.Correspondingly, adopt AB of the present invention
5The Ni-MH battery that the type cathode hydrogen storage material prepares has good low temperature charge-discharge performance, and has characteristics such as broad application temperature range.
Description of drawings
Fig. 1 shows low temperature capacity (40～30 ℃) test result of the hydrogen bearing alloy of hydrogen bearing alloy of the present invention and prior art.
Embodiment
Below in conjunction with embodiment the present invention is launched to further describe.But should be appreciated that following execution mode only is used for the present invention is illustrated and is not in order to limit scope of the present invention.
According to alloy A in the table 2
1B
5The percentage by weight of each element is prepared burden, and the alloy raw material for preparing is carried out melting and ingot casting in the induction furnace that vacuumizes afterwards and feed argon shield, waits to obtain to become stand-by less than 200 purpose alloyed powders in grinding at room temperature behind the as cast condition hydrogen bearing alloy.
The composition of table 2 embodiment of the invention and prior art is (wt%) relatively
| Composition | La | Ce | Pr | Nd | Ga | Ni | Co | Mn | Al | |
| The present invention | MmNi 3.50Ga 0.05Co 0.75Mn 0.4Al 0.3 | 21.80 | 7.60 | 0.99 | 2.64 | 0.82 | 48.58 | 10.45 | 5.20 | 1.91 |
| MmNi 3.45Ga 0.10Co 0.75Mn 0.4Al 0.3 | 21.77 | 7.59 | 0.99 | 2.64 | 1.65 | 47.82 | 10.44 | 5.19 | 1.91 | |
| MmNi 3.40Ga 0.15Co 0.75Mn 0.4Al 0.3 | 21.74 | 7.58 | 0.99 | 2.64 | 2.47 | 47.07 | 10.43 | 5.18 | 1.91 | |
| MmNi 3.35Ga 0.20Co 0.75Mn 0.4A1 0.3 | 21.72 | 7.57 | 0.99 | 2.63 | 3.28 | 46.32 | 10.41 | 5.18 | 1.91 | |
| MmNi 3.30Ga 0.25Co 90.75Mn 0.4Al 0.3 | 21.69 | 7.56 | 0.99 | 2.63 | 4.10 | 45.57 | 10.40 | 5.17 | 1.90 | |
| MmNi 3.25Ga 0.30Co 0.75Mn 0.4Al 0.3 | 21.66 | 7.55 | 0.98 | 2.63 | 4.91 | 44.82 | 10.39 | 5.16 | 1.90 | |
| Comparative Examples | MmNi 3.55Co 0.75Mn 0.4Al 0.3 | 21.83 | 7.61 | 0.99 | 2.65 | 0.00 | 49.34 | 10.47 | 5.20 | 1.92 |
The method of testing of electrochemistry capacitance is as follows: will be less than 200 purpose negative alloy powders and the nickel powder mixed by 1: 1, and add an amount of poly-vinyl alcohol solution as binding agent, be cold-pressed into diameter then and use [the Ni (OH) that used positive electricity is very identical with Ni-MH battery as negative electrode for the cake of (d=15mm)
2-NiOOH] electrode, the Capacity design of positive electrode is the capacity far above negative electrode, so that negative electrode material reaches fully saturated when charging, [Hg/HgO/6M KOH] is reference electrode.In the electrode performance test process, at first adopt the electric current of 60mA/g that storage hydrogen negative material is fully changed at 30 ℃, the system that changes into is as follows: the current charges 400min that adopts 60mA/g, paused 15 minutes in the charging back, till being-0.5 volt to the negative electrode current potential with respect to the electrode potential of reference electrode with the current discharge of 60mA/g then, carry out the next round charge and discharge cycle again.Capacity of negative plates carries out capacity and will reach a maximum along with what change into, and relatively stablely gets off, and then changes into end.This maximum is the hydrogen storage capability of material under 30 ℃, reduces system temperature then, adopts the identical hydrogen storage capability of charge and discharge system test negative material under different temperatures in 30～-40 ℃ of scopes.
The AB of each execution mode of the present invention (different Ge content) that said method is recorded
5The discharge capacity test result drafting pattern of type hydrogen storage material under different temperatures, as shown in Figure 1.In addition, for ease of relatively, also will adopt the AB of each execution mode of the present invention (different Ge content) that said method records
5Traditional AB of type hydrogen storage material and prior art
5The discharge capacity of type hydrogen storage material under different temperatures listed in the table 3.
The discharge capacity (mAh/g) of table 3 hydrogen bearing alloy under different temperatures
By the data of the curve tendency of Fig. 1 and table 3 as can be known: each cast alloy capacity is suitable substantially in the time of 30 ℃, but reduces with temperature, and all alloy capacity all reduce gradually, and the amplitude of reduction is different with the variation of alloying component.Under same temperature, along with the increase of alloying component Ga content, promptly x changes to 0.3 from 0.05, and the low temperature capacity of alloy is increases the trend that afterwards reduces earlier, and (weight content of corresponding Ga is 4.10wt%) cryogenic property is best when x=0.25.These alloys that contain the Ga element and Ga content are that 0 Comparative Examples is compared, and capacity improves, and temperature is low more, the amplitude that capacity improves is big more, and particularly during lower temperature, capacity can be by 10mAh/g (x=0 during as-40 ℃, 0.0wt%Ga) bring up to 203mAh/g (x=0.25,4.10wt%Ga).Therefore, the adding of Ga can make the low temperature electrochemical charge/discharge capacity of alloy obviously improve, and it is best in Ga content x=0.25 (percentage by weight is 4.10%) performance, electrochemistry charge and discharge capacity when resulting best result is-30 ℃ is 252mAh/g, the charge and discharge capacity reaches 203mAh/g in the time of-40 ℃, therefore will make this negative material use the stronger advantage that has at low temperatures.
In sum, the Ni-based hydrogen bearing alloy MmNi of mishmetal
3.55-xGa
xCo
0.75Mn
0.4Al
0.3When the low temperature charge-discharge performance, particularly temperature of the content influence alloy of middle Ga element was low, the charge and discharge capacities chart revealed certain raising.That is to say, add metal Ga in hydrogen bearing alloy, can obtain the negative material that the good suitable low temperature nickel hydrogen battery of cryogenic property uses.This material possesses the higher charge and discharge capacity apparently higher than commercially available hydrogen bearing alloy in 30～-40 ℃ of scopes, the electrochemistry charge and discharge capacity in the time of its-30 ℃ is greater than 250mAh/g, and capacity reaches 203mAh/g in the time of-40 ℃.In addition, AB of the present invention
5Type cathode hydrogen storage material---MmNi
3.55-xGa
xCo
0.75Mn
0.4Al
0.3(0＜x≤0.3) also has characteristics such as broad application temperature range.
Claims (6)
1. AB
5The type cathode hydrogen storage material, its atomic ratio composition consists of MmNi
3.55-xGa
xCo
0.75Mn
0.4Al
0.3, 0＜x≤0.3 wherein, Mm is the lucium of being made up of La, Ce, Pr, Nd element, and the total weight with lucium Mm is a benchmark, and the content of La is 64.5-67.5%, and the content of Ce is 22.0-24.0%, the content of Pr is 2.5-3.5%, and the content of Nd is 7.0-9.0%.
2. AB according to claim 1
5The type cathode hydrogen storage material is characterized in that, 0.15≤x≤0.3.
3. AB according to claim 1
5The type cathode hydrogen storage material is characterized in that, described AB
5The atomic ratio composition of type cathode hydrogen storage material consists of:
MmNi
3.50Ga
0.05Co
0.75Mn
0.4Al
0.3；
MmNi
3.45Ga
0.10Co
0.75Mn
0.4Al
0.3；
MmNi
3.40Ga
0.15Co
0.75Mn
0.4Al
0.3；
MmNi
3.35Ga
0.20Co
0.75Mn
0.4Al
0.3；
MmNi
3.30Ga
0.25Co
0.75Mn
0.4Al
0.3Or
MmNi
3.25Ga
0.30Co
0.75Mn
0.4Al
0.3。
4. AB according to claim 3
5The type cathode hydrogen storage material is characterized in that, described AB
5The atomic ratio composition of type cathode hydrogen storage material consists of:
MmNi
3.30Ga
0.25Co
0.75Mn
0.4Al
0.3。
5. the described AB of claim 1
5The application of type cathode hydrogen storage material in the preparation nickel-hydrogen battery negative pole.
6. application according to claim 5 is characterized in that, described Ni-MH battery is to be suitable for the Ni-MH battery that low temperature discharges and recharges.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB2005100999026A CN100372157C (en) | 2005-09-09 | 2005-09-09 | AB5 type negative pole hydrogen-storage material |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB2005100999026A CN100372157C (en) | 2005-09-09 | 2005-09-09 | AB5 type negative pole hydrogen-storage material |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1738084A true CN1738084A (en) | 2006-02-22 |
| CN100372157C CN100372157C (en) | 2008-02-27 |
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CNB2005100999026A Expired - Fee Related CN100372157C (en) | 2005-09-09 | 2005-09-09 | AB5 type negative pole hydrogen-storage material |
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|---|---|
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113166853A (en) * | 2018-12-04 | 2021-07-23 | 株式会社三德 | Hydrogen storage material, negative electrode and nickel-hydrogen secondary battery |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP3730265B2 (en) * | 1994-04-01 | 2005-12-21 | 株式会社東芝 | Hydrogen storage alloy for battery, manufacturing method thereof and nickel metal hydride battery |
| CN1093691C (en) * | 1996-01-15 | 2002-10-30 | 中国科学院金属研究所 | Hydrogen-absorption alloy gold powder for electrode |
| CN1294664C (en) * | 2004-06-03 | 2007-01-10 | 刘华福 | Negative hydrogen storage material for high-temperature nickel hydrogen battery |
-
2005
- 2005-09-09 CN CNB2005100999026A patent/CN100372157C/en not_active Expired - Fee Related
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113166853A (en) * | 2018-12-04 | 2021-07-23 | 株式会社三德 | Hydrogen storage material, negative electrode and nickel-hydrogen secondary battery |
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| Publication number | Publication date |
|---|---|
| CN100372157C (en) | 2008-02-27 |
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