CN102983368B - Preparation method of high-temperature NI-MH power battery - Google Patents
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Abstract
The invention relates to a preparation method of a high-temperature NI-MH power battery, in particular relates to a production technique for the NI-MH power battery with excellent high-temperature property, and belongs to the field of secondary battery preparation technologies. In the manufacturing process of the battery, secondary coating is conducted to the surface of a nickel electrode with graphene pulp by utilizing the characteristics of graphene, and pretreating is conducted to a negative electrode skeleton so as to fully form a three-dimensional conductive network. Therefore, the conductivity of the electrode can be increased, the charging receiving capability of the electrode under high-temperature condition can be improved, the electrochemical activity of active materials and oxygen evolution potential of a positive electrode can be enhanced, the problems that a NI-MH battery as a power battery is low in high-temperature charging efficiency and heats in large-current charging can be overcome, and the NI-MH power battery with excellent high-temperature charging property, excellent high-rate discharging property and long recycling life can be prepared.
Description
Technical field
The present invention relates to a kind of preparation method of high temperature Ni-MH power cell, be specifically related to the manufacturing process of the Ni-MH power cell that a kind of high-temperature behavior is good, belong to secondary cell preparing technical field.
Background technology
Ni-MH battery is with features such as its good charge-discharge performance, pollution-free, high power capacity and high-energy-densities, from the nineties industrialization in the last century history of existing ten several years so far, is the leading products in secondary cell market always.Not only be widely used in all kinds of consumer electronic product, but also be used as the first-selected product of electric vehicle power sources.
The electric equipment products emerging in an endless stream, usually needs battery (>=45 ℃) work under higher ambient temperature.Rechargeable battery is in charge and discharge process, and it is huge that the variation of ambient temperature exerts an influence to battery performance.Traditional Ni-MH battery is when serviceability temperature surpasses 30 ℃, and its charge efficiency can decline along with the rising of temperature, and battery is at high temperature used also can cause hydraulic performance decline, and decay is accelerated.
Therefore for a long time, the research of researching high-temperature ni-mh was never interrupted.Except disclosing anticathode hydrogen-storage alloy, a few patents adds lanthanum, cerium, polonium, vanadium, iron, nickel, zinc, tungsten, chromium, titanium, one or more oxides in lithium, beyond hydroxide improves, major technique is still positive electrode, being included in battery village material formula takes mechanical mixing to add rare earth, rare metal, alkaline earth element is as magnesium, calcium, strontium, Cerium, ytterbium, lanthanum, lanthanide series, because positive pole batching is difficult to reach completely evenly, so some considerations adopt the coprecipitation above-mentioned element that adulterates during fabrication, also there is the hydroxide of considering the coated above-mentioned element of one deck on ball nickel.Although above-mentioned several method has certain effect to improving high-temperature battery performance, but still exist many deficiencies, although coated, above-mentioned phenomenon is had to certain improvement, but still exist coated firm not, after discharging and recharging, occur that superficial layer dissolves and obscission, make active material loss, conductivity reduces, and has a strong impact on cycle life and efficiency.
Another kind method is to add cobalt protoxide and cobalt hydroxide, but in its charge and discharge process after interpolation, Yi Bian be dissolved in alkaline aqueous solution, separate out again again on one side, and structural change sharply occurs, have part cobalt compound free, thereby cause cobalt quantitative change to cause battery performance to reduce
Graphene is a kind of carbonaceous new material of the tightly packed one-tenth individual layer of carbon atom bi-dimensional cellular shape lattice structure, is the elementary cell that builds other dimension carbonaceous material (as zero dimension fullerene, one-dimensional nano carbon pipe, three-dimensional graphite).Its thickness only has 0.335 nanometer, be only 200,000 of hair/, the theoretical specific area of Graphene is up to 2600m
2, Pg has outstanding heat conductivility (3000Wm
-1k
-1)) and mechanical property (1060GPa), and normal temperature and above higher electron mobility (15000cm
2v
-1s
-1).
Graphene is the material with carbon element that is the netted bonding of hexagon, has a lot of outstanding electrical characteristics.Carbon atom has four valence electrons, and each carbon atom is contributed a not Cheng Jian like this
πelectronics, these
πelectronics becomes vertical direction can form track with plane,
πelectronics can move freely in crystal, gives the conductivity that Graphene is good.The patience to high current density considerably beyond copper.
Compare with other materials, Graphene also has much very special character.Though Graphene does not much find out that principle is but considered to very promising application examples in addition.Such as the electrode material as Li-Ion rechargeable battery.By adding a small amount of Graphene in the electrode to Li-Ion rechargeable battery, not only can keep original energy density, also can significantly improve output power density.Graphene also has the advantages such as environmental protection and energy saving.Will be in energy industry great Zhan advantage.
Summary of the invention
The object of the invention is to overcome the shortcoming that secondary Ni-MH battery charge efficiency declines along with the rising of temperature and high current charge-discharge generates heat, Ni-MH power cell of high current charge-discharge under a kind of applicable hot environment and preparation method thereof is provided.
According to technical scheme provided by the invention, the present invention is according to the netted bonding structure of Graphene, ultra-thin thickness and huge specific area, the feature of high conductivity and heat conduction, at the anodal secondary of nickel, be coated with the Graphene slurry of carrying out two-dimensional nanostructure, to form three-dimensional conductive network on anodal surface, improve nickel electrode at high temperature charge acceptance improve the overpotential for oxygen evolution of battery, improve the efficiency for charge-discharge of large electric current, thereby in minimizing system because oxygen produces, compound and the thermal effect that causes, the internal resistance of reduction system, reduce electrochemical polarization, concentration polarization and ohmic polarization, reduce the generation of corresponding heat.Greatly improved on the one hand the high-temperature behavior of nickel electrode: also help the performance of the anodal energy of nickel simultaneously, do high-rate discharge ability, extending battery life, reduces conductive agent consumption.
A preparation method for high temperature Ni-MH power cell, step following steps are as follows by weight for formula rate:
(1) preparation of nickel slurry: get 1.5 ~ 5.5 parts of adhesives and 30 ~ 50 parts of pure water, beat glue 2 ~ 6h with the rotating speed of 150 ~ 300r/min; Add 1 ~ 3 part of additive of 36.5 ~ 64.5 parts of positive active materials and 2 ~ 5 parts of conductive agents, rotating speed stirring 3 ~ 5 h with 100 ~ 300r/min, obtain nickel slurry;
(2) coating is dry: get the nickel slurry that step (1) makes and be coated on anodal skeleton, coating layer thickness is 1.0 ~ 1.5mm, after be coated with, as for the baking oven inner drying 0.5 ~ 1h of 80 ~ 150 ℃, nickel slurry is dried, the nickel-base anode that obtains being once coated with;
(3) preparation of Graphene slurry: get 1 ~ 5 part of adhesive and 20 ~ 40 parts of pure water, beat glue 2 ~ 6 h with the rotating speed of 150 ~ 300r/min; Add 40 ~ 60 parts of Graphenes and 1 ~ 4 part of graphene dispersing solution, after the rotating speed stirring 20 ~ 60min with 100 ~ 300r/min, pack ball grinder into and carry out ball milling dispersion with ball mill, to viscosity be 3000 ~ 4000cP, add 1 ~ 6 part of pure water, being adjusted to viscosity is 1000 ~ 2100cP again, obtains Graphene slurry;
(4) secondary coating is dry: get Graphene slurry prepared by step (3) the once nickel-base anode of coating of step (2) gained is carried out to secondary coating, coating thickness is 0.008 ~ 0.028mm, after being coated with as for the baking oven inner drying 0.3 ~ 1h of 60 ~ 100 ℃, make nickel slurry dry, obtain the anodal substrate of nickel, last itemize, cut-parts, spot welding lug, obtain tweezer positive pole;
(5) battery cathode sheet preparation: get hydrogen-bearing alloy powder by powder on starching machine on negative pole skeleton, upper powder thickness is 0.4 ~ 0.8mm, then, by the roll-in of pressure roller normal temperature, pressure is 1500 ~ 3000MPa, after pressing, the density of hydrogen-bearing alloy powder is 1.5 ~ 3.5g/cm
3; Negative pole skeleton after pressing is soaked to ptfe emulsion, flood after 1 ~ 5 second in 60 ~ 80 ℃ of oven dry, section, obtain battery cathode sheet;
(6) preparation of high temperature Ni-MH power cell: get anodal and step (5) the gained battery cathode sheet of step (4) gained tweezer and by membrane coil, be coiled into electric stamen and pack in nickel plating box hat, the block of burn-oning, injection electrolyte, seals and obtains product high temperature Ni-MH power cell.
Described adhesive is the mixture of one or more materials in sodium carboxymethylcellulose, hydroxypropyl methylcellulose, butadiene-styrene rubber or polytetrafluoroethylene.Described positive active material is ball-type hickelous nydroxide.
Described anodal skeleton is a kind of in nickel foam and nickel plating perforated steel ribbon.
Described additive is the mixture of one or more materials in the sub-cobalt of hydrogen hydrogenation, cobalt protoxide, yttria or calcium; Described conductive agent is the mixture of one or more materials in active carbon, carbon black, acetylene carbon black, super carbon black Super-P, graphite, polyaniline or polyacetylene.
Described negative pole skeleton is that copper mesh grid or copper are cut a kind of in drawing in the net.
Described negative electrode active material is AB5 type low-cobalt hydrogen storage alloy powder.
Described Graphene is the netted bonded carbon material of individual layer or the hexagon of the number of plies between 3-15 layer; Be specially one or more the mixture in Ni-based, copper base, silica-based and carboxylated Graphene, amination Graphene, sulfhydrylation Graphene, graphene oxide.
Described graphene dispersing solution adopts polarity or nonpolar graphene dispersing solution to disperse.
The described barrier film of step (6) is to take sulfonated membrane that polypropylene material is matrix or fluoridize barrier film; Described electrolyte is the ternary electrolyte of NaOH, potassium hydroxide and lithium hydroxide.
The present invention goes back anticathode skeleton and carries out the preliminary treatment of Graphene coating.This coating as thin as a wafer, does not reduce battery specific energy, and the adhesive force between enhanced activity layer and collector reduces interface resistance, improves battery high rate performance, reduces and stable cell internal resistance raising multiplying power cycle life.
Tool of the present invention has the following advantages: the present invention improves the charge efficiency under hot conditions, carries high-rate charge-discharge capability, reduces the interpolation of conductive agent, has improved the energy content of battery, has also extended the cycle life of battery.
Embodiment
Embodiment 1
(1) preparation of nickel slurry: get 4 parts of adhesive C MC and 45 parts of pure water, beat glue 4h with the rotating speed of 200r/min; Add 64.5 parts of positive active material ball-type hickelous nydroxides, 3 parts of additive cobalt protoxides and 4 parts of conductive agent active carbons, rotating speed stirring 3 ~ 5 h with 100 ~ 300r/min, obtain nickel slurry;
(2) coating is dry: get the nickel slurry that step (1) makes and be coated on anodal skeleton, coating layer thickness is 1.0mm, after be coated with, as for the baking oven inner drying 0.5h of 150 ℃, nickel slurry is dried, the nickel-base anode that obtains being once coated with;
(3) preparation of Graphene slurry: get 3 parts of adhesive HPMC and 40 parts of pure water, beat glue 4h with the rotating speed of 200r/min; Add 60 parts of few layer graphenes and 1 part of nonpolar graphene dispersing solution, after the rotating speed stirring 60min with 100r/min, pack ball grinder into and carry out ball milling dispersion with ball mill, to viscosity be 3000cP, add 6 parts of pure water, being adjusted to viscosity is 1000cP again, obtains Graphene slurry;
(4) secondary coating is dry: get Graphene slurry prepared by step (3) the once nickel-base anode of coating of step (2) gained is carried out to secondary coating, coating thickness is 0.008mm, after being coated with as for the baking oven inner drying 1h of 100 ℃, make nickel slurry dry, obtain the anodal substrate of nickel, last itemize, cut-parts, spot welding lug, obtain tweezer positive pole;
(5) battery cathode sheet preparation: get hydrogen-bearing alloy powder by powder on starching machine on negative pole skeleton, upper powder thickness is 00.6mm, then, by the roll-in of pressure roller normal temperature, pressure is 2000MPa, after pressing, the density of hydrogen-bearing alloy powder is 1.5 ~ 3.5g/cm
3; Negative pole skeleton after pressing is soaked to ptfe emulsion, flood after 1 ~ 5 second in 60 ~ 80 ℃ of oven dry, section, obtain battery cathode sheet;
(6) preparation of high temperature Ni-MH power cell: get anodal and step (5) the gained battery cathode sheet of step (4) gained tweezer and by membrane coil, be coiled into electric stamen and pack in nickel plating box hat, the block of burn-oning, injection electrolyte, seals and obtains products A A type cylindrical nickel-metal hydride battery.
After tested, 40 ℃ of 1C fill 70 minutes, and discharge capacity is that 91.%, 70 ℃ of 1C of normal temperature capacity charges 70 minutes, and discharge capacity is 83% of normal temperature capacity, circulate 150 times, and capacity attenuation 12%
Embodiment 2
Method preparation by identical with embodiment 1, is just increased to 0.012mm by the thickness of anodal secondary coating.After tested, 45 ℃ of 1C fill 70 minutes, and discharge capacity is that 94.1%, 70 ℃ of 1C of normal temperature capacity fills 70 minutes, and discharge capacity is 86.4% of normal temperature capacity, and capability retention 81.2% after 350 times circulates.
Embodiment 3
By the method preparation identical with embodiment 2, wherein in step (1), adhesive C MC adds 5.5 parts, and positive active material ball-type hickelous nydroxide adds 55 parts, 3 parts of conductive agent active carbons; After tested, normal temperature 1C capacity has improved 17mAh.40 ℃ and 70 ℃ of efficiency for charge-discharges do not have to change substantially.
Embodiment 4
By the method preparation identical with embodiment 1, in the preparation of step (5) battery cathode sheet, first negative pole skeleton copper mesh is graphited alkene slurry coating, oven dry, then adopt dry compression mode, hydrogen-bearing alloy powder is colded pressing on copper mesh after by powder on starching machine, then soak PTFE emulsion, oven dry, section, make negative plate.Other technique is constant.
After tested, 40 ℃ of 1C fill 70 minutes the battery of making, and discharge capacity is that 95.7%, 70 ℃ of 1C of normal temperature capacity charges 70 minutes, and discharge capacity is 88.3% of normal temperature capacity, circulate 230 times, and capacity attenuation 14%.
Embodiment 5
Method preparation by identical with embodiment 4, just will just be increased to 0.022mm by the thickness of anodal secondary coating.After tested, 40 ℃ of 1C charge efficiencies and 70 ℃ of 1C charge efficiencies have improved respectively 1.4% and 1.7%, and the capacity after 100 times that circulates keeps not changing substantially.
Comparative example 1
By the weight ratio of 4:93:3, take adhesive C MC, positive active material ball-type hickelous nydroxide and additive cobalt protoxide, first with CMC and pure water, play glue, then add positive active material ball-type hickelous nydroxide and additive cobalt protoxide to stir and make nickel slurry, then be coated on nickel foam skeleton, itemize, cut-parts, spot welding lug after oven dry, spreading, make nickel positive pole.
Negative pole adopts dry process mode to prepare, and is that hydrogen-bearing alloy powder is colded pressing on copper mesh by powder on starching machine again, then soaks PTFE emulsion glue, oven dry, section, makes negative plate.
Then by the positive/negative plate of making and PP polypropylene non-woven fabric membrane coil, be coiled into electric stamen and pack nickel plating box hat into, add potassium hydroxide and lithium hydroxide binary electrolyte again, AA type cylinder nickel-hydrogen secondary cell is made in sealing.
After tested, normal temperature capacity is normal, and 40 ℃ of 1C charge efficiencies and 70 ℃ of 1C charge efficiencies only have respectively 83.5% and 45.0%.
The present invention is only suitable in nickel-hydrogen secondary cell, positive and negative plate and barrier film and the electrolyte structure by this technique, made; Collector includes but not limited to the electric conducting materials such as copper, nickel.It can be the form such as foam, net, paper tinsel of metal.
Claims (10)
1. a preparation method for high temperature Ni-MH power cell, step following steps are as follows by weight to it is characterized in that formula rate:
(1) preparation of nickel slurry: get 1.5 ~ 5.5 parts of adhesives and 30 ~ 50 parts of pure water, beat glue 2 ~ 6h with the rotating speed of 150 ~ 300r/min; Add 36.5 ~ 64.5 parts of positive active materials, 1 ~ 3 part of additive and 2 ~ 5 parts of conductive agents, rotating speed stirring 3 ~ 5 h with 100 ~ 300r/min, obtain nickel slurry;
(2) coating is dry: get the nickel slurry that step (1) makes and be coated on anodal skeleton, coating layer thickness is 1.0 ~ 1.5mm, be coated with the baking oven inner drying 0.5 ~ 1h that is placed on 80 ~ 150 ℃, nickel slurry is dried, the nickel-base anode that obtains being once coated with;
(3) preparation of Graphene slurry: get 1 ~ 5 part of adhesive and 20 ~ 40 parts of pure water, beat glue 2 ~ 6 h with the rotating speed of 150 ~ 300r/min; Add 40 ~ 60 parts of Graphenes and 1 ~ 4 part of graphene dispersing solution, after the rotating speed stirring 20 ~ 60min with 100 ~ 300r/min, pack ball grinder into and carry out ball milling dispersion with ball mill, to viscosity be 3000 ~ 4000cP, add 1 ~ 6 part of pure water, being adjusted to viscosity is 1000 ~ 2100cP again, obtains Graphene slurry;
(4) secondary coating is dry: get Graphene slurry prepared by step (3) the once nickel-base anode of coating of step (2) gained is carried out to secondary coating, coating thickness is 0.008 ~ 0.028mm, be coated with the baking oven inner drying 0.3 ~ 1h that is placed on 60 ~ 100 ℃, make Graphene slurry dry, obtain the anodal substrate of nickel, last itemize, cut-parts, spot welding lug, obtain nickel positive pole;
(5) battery cathode sheet preparation: get hydrogen-bearing alloy powder by powder on starching machine on negative pole skeleton, upper powder thickness is 0.4 ~ 0.8mm, then, by the roll-in of pressure roller normal temperature, pressure is 1500 ~ 3000MPa, after pressing, the density of hydrogen-bearing alloy powder is 1.5 ~ 3.5g/cm
3; Negative pole skeleton after pressing is soaked to ptfe emulsion, flood after 1 ~ 5 second in 60 ~ 80 ℃ of oven dry, section, obtain battery cathode sheet;
(6) preparation of high temperature Ni-MH power cell: get anodal and step (5) the gained battery cathode sheet of step (4) gained nickel and by membrane coil, be coiled into battery core and pack in nickel plating box hat, the block of burn-oning, injection electrolyte, seals and obtains product high temperature Ni-MH power cell.
2. the preparation method of high temperature Ni-MH power cell as claimed in claim 1, is characterized in that: described adhesive is the mixture of one or more materials in sodium carboxymethylcellulose, hydroxypropyl methylcellulose, butadiene-styrene rubber or polytetrafluoroethylene.
3. the preparation method of high temperature Ni-MH power cell as claimed in claim 1, is characterized in that: described positive active material is ball-type hickelous nydroxide.
4. the preparation method of high temperature Ni-MH power cell as claimed in claim 1, is characterized in that: described anodal skeleton is a kind of in nickel foam and nickel plating perforated steel ribbon.
5. the preparation method of high temperature Ni-MH power cell as claimed in claim 1, is characterized in that: described additive is the mixture of one or more materials in the sub-cobalt of hydrogen hydrogenation, cobalt protoxide, yttria or calcium;
Described conductive agent is the mixture of one or more materials in active carbon, carbon black, graphite, polyaniline or polyacetylene.
6. the preparation method of high temperature Ni-MH power cell as claimed in claim 1, is characterized in that: described negative pole skeleton is that copper mesh grid or copper are cut a kind of in drawing in the net.
7. the preparation method of high temperature Ni-MH power cell as claimed in claim 1, is characterized in that: described negative electrode active material is AB
5type low-cobalt hydrogen storage alloy powder.
8. the preparation method of high temperature Ni-MH power cell as claimed in claim 1, is characterized in that: described Graphene is the netted bonded carbon material of individual layer or the hexagon of the number of plies between 3-15 layer; Be specially one or more the mixture in Ni-based, copper base, silica-based and carboxylated Graphene, amination Graphene, sulfhydrylation Graphene, graphene oxide.
9. the preparation method of high temperature Ni-MH power cell as claimed in claim 1, is characterized in that: described graphene dispersing solution adopts polarity or nonpolar graphene dispersing solution to disperse.
10. the preparation method of high temperature Ni-MH power cell as claimed in claim 1, is characterized in that: the described barrier film of step (6) is to take sulfonated membrane that polypropylene material is matrix or fluoridize barrier film; Described electrolyte is the ternary electrolyte of NaOH, potassium hydroxide and lithium hydroxide.
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| CN106340682A (en) * | 2016-10-31 | 2017-01-18 | 河南创力新能源科技股份有限公司 | Nickel-metal hydride battery electrolyte additive, electrolyte containing additive and nickel-metal hydride battery |
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| CN104157865B (en) * | 2014-06-17 | 2016-03-02 | 安徽亿诺新能源有限责任公司 | A kind of nickel-hydrogen battery positive pole material |
| CN104269532B (en) * | 2014-09-05 | 2017-01-11 | 广东工业大学 | Preparation method of negative pole of graphene-based high-capacity nickel-hydrogen power battery |
| CN106898761B (en) * | 2017-05-02 | 2019-09-17 | 卢国骥 | The electrode sheet material preparation process and graphene nickel-zinc cell of graphene nickel-zinc cell |
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| CN109546091B (en) * | 2018-11-07 | 2021-10-26 | 超威电源集团有限公司 | Preparation method of high-specific-energy zinc-nickel battery positive electrode |
| CN114914556A (en) * | 2022-03-23 | 2022-08-16 | 东莞超霸电池有限公司 | Nickel-hydrogen battery and preparation method thereof |
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| CN102496480B (en) * | 2011-12-16 | 2013-09-18 | 江南大学 | Preparation method of graphene/nickel-aluminum bi-metal hydroxide composite material and application thereof |
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Effective date of registration: 20191212 Address after: 231400 innovation and entrepreneurship Industrial Park, Dongyi Road Economic Development Zone, Tongcheng economic and Technological Development Zone, Anqing City, Anhui Province Patentee after: Tongcheng Chaoxiang Network Technology Co.,Ltd. Address before: 231300 Shucheng economic and Technological Development Zone, Anhui, Lu'an Patentee before: ANHUI INNOVATION NEW ENERGY Co.,Ltd. |
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Effective date of registration: 20230224 Address after: 235300 south of the intersection of Zhoushi road and Liuba Road, Sunji village, Zhouzhai Town, Dangshan County, Suzhou City, Anhui Province Patentee after: Dangshan Nafang packaging material Co.,Ltd. Address before: 231400 Innovation and Entrepreneurship Industrial Park, Dongyi Road, Economic and Technological Development Zone, Tongcheng City, Anqing City, Anhui Province Patentee before: Tongcheng Chaoxiang Network Technology Co.,Ltd. |