CN103050700A - Positive electrode material for lithium-air battery or lithium-oxygen battery - Google Patents
Positive electrode material for lithium-air battery or lithium-oxygen battery Download PDFInfo
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- CN103050700A CN103050700A CN2011103147837A CN201110314783A CN103050700A CN 103050700 A CN103050700 A CN 103050700A CN 2011103147837 A CN2011103147837 A CN 2011103147837A CN 201110314783 A CN201110314783 A CN 201110314783A CN 103050700 A CN103050700 A CN 103050700A
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Abstract
The invention relates to a positive electrode material for a lithium-air battery or lithium-oxygen battery. The positive electrode material comprises two or three carbon materials, wherein under the operation conditions of a battery, the carbon material A is poorer in wettability to an electrolyte solution and has a contact angle with the electrolyte solution between 105 DEG and 170 DEG, the carbon material B is proper in wettability to the electrolyte solution and has a contact angle with the electrolyte solution between 70 DEG and 110 DEG, and the carbon material C is better in wettability to the electrolyte solution and has a contact angle with the electrolyte solution between 10 DEG and 70 DEG. According to the positive electrode material provided by the invention, because a lyophilic carbon material or lyophobic carbon material is mixed, an electrode is fully wetted by the electrolyte solution, so that a maximum solid-liquid two-phase reaction interface is obtained, the transfer of oxygen in the electrode is improved, the utilization rate of the reaction interface is increased, and then the charge and discharge capacity of the battery is improved.
Description
Technical field
The present invention relates to a kind of lithium-air battery or lithium-aeration cell critical material field, be specifically related to a kind of lithium-air battery or lithium-aeration cell positive electrode.
Background technology
Lithium-air battery is a kind of take lithium metal as negative pole, air electrode is anodal rechargeable type secondary cell, lithium metal as negative material has minimum theoretical voltage, its theoretical specific capacity is up to 3,862mAh/g, and can directly from air, obtain as the oxygen of positive active material, therefore, lithium-air battery has high specific capacity and specific energy.Take lithium as standard, its theoretical specific energy density can reach 11,140Wh/Kg, and take full battery as standard, its actual specific energy density is about 10 times of lithium ion battery, has application prospect in civilian and military domain.The specific energy that following business-like pure electric vehicle requires electrokinetic cell more than 500Wh/kg, scientist lithium-air battery as one of electrokinetic cell of following electric automobile.
Fig. 1 by anodal in the lithium-air battery discharge process and the schematic diagram of generation electrochemical reaction.As shown in the figure, the oxygen composition generation product Li that the lithium ion that is arrived by negative side migration arrives in carbon material surface and diffusion
2O
2Perhaps Li
2O.Solid Li
2O
2Perhaps Li
2O is insoluble to electrolyte solution, can not break away from carbon material surface, thus in this deposition until stop up electrode duct, guiding discharge reaction terminating.At present, lithium-air battery anode reactant mass transfer situation generally adopts solid-liquid two phase reaction INTERFACE MODEL to explain, the interface that namely forms between solid-material with carbon element and the liquid-electrolyte solution, and wherein material with carbon element is responsible for conduction electron, and electrolyte is responsible for conducting Li
+, extraneous oxygen arrives reaction interface through the diffusion of the dissolving in electrolyte solution, finishes exoelectrical reaction Li at these reaction three elements
++ O
2-e → Li
2O
2Perhaps Li
++ O
2-e → Li
2O.
In order to obtain larger solid-liquid two phase reaction interface and more unobstructed Li
+Conduction pathway requires electrolyte solution higher to the infiltration degree of electrode, and the material with carbon element that namely consists of electrode has preferably lyophily.But then, because the dissolving diffusivity of oxygen in electrolyte solution is relatively poor, if electrode is infiltrated by electrolyte fully, then the resistance to mass tranfer of oxygen in electrode is larger, especially for electrode inboard (namely away from air side), therefore, require to exist in the electrode more unobstructed gas delivery passage, make oxygen fully diffusion in whole electrode, shorten it to the distance of carbon material surface (being solid-liquid two phase reaction interface) diffusion, reduce its resistance to mass tranfer, this has preferably lyophobicity with regard to the material with carbon element that requires to consist of electrode.Yet a kind of material with carbon element can not possess above-mentioned two specific characters simultaneously, namely good electrolyte wettability and preferably gas transfer can not get both.
Summary of the invention
The present invention is directed to the problems referred to above, a kind of Novel lithium-air or lithium-aeration cell positive electrode are provided, purpose is to improve electrolyte to infiltration and the mass transfer situation of oxygen in electrode of electrode.
As the material with carbon element of electrode body material, it is to electrolyte or have preferably wettability, perhaps has stronger lyophobicity, perhaps between between the two.In order to guarantee that electrolyte forms good infiltration to obtain larger solid-liquid two phase reaction interface and more unobstructed Li to electrode
+Conduction pathway, guarantee simultaneously to have more unobstructed gas delivery passage in the electrode, for the different physical property of electrode body material with carbon element, the present invention sneaks into the stronger material with carbon element of lyophily respectively in electrode, the perhaps stronger material with carbon element of lyophobicity, perhaps two kinds of material with carbon elements are all sneaked into.The material with carbon element of sneaking into both can be used as the place that electrode reaction is carried out, simultaneously according to the difference of its physical property, can be respectively as the transmission channel of electrolyte and gas.By said method, increased the reaction interface area, strengthen the transmission of electrode reaction thing, thereby be conducive to improve the charge/discharge capacity of battery.
For achieving the above object, the technical solution used in the present invention is:
Positive electrode of the present invention comprises two or three material with carbon element; Under the battery operation condition:
Material with carbon element A be to the electrolyte solution wettability relatively poor, and the contact angle of electrolyte solution between the 105-170 degree;
Material with carbon element B be the wettability to electrolyte solution moderate, and the contact angle of electrolyte solution between the 70-110 degree;
Material with carbon element C for electrolyte solution is had preferably infiltrating, and the contact angle of electrolyte solution between the 10-70 degree;
When comprising two kinds of material with carbon elements, positive electrode is A+B, wherein A: the B mass ratio is 0.05～10: 1; Or C+B, wherein C: the B mass ratio is 0.05～10: 1; Or A+C, wherein A: the C mass ratio is 0.05～20: 1;
When comprising three kinds of material with carbon elements, positive electrode is A+B+C, and wherein the mass fraction of B is 30-90%, A: the C mass ratio is 0.05～20: 1.
Described material with carbon element is carbon nanomaterial, such as KB600, Super P, Super S, BP2000, XC-72, Denka Black, KB300, ENSACO 350G, Printex XE2, Printex XE2-B, Alkaline-activated carbon, Maxsorb 1470, Maxsorb 2400, Maxsorb 3100, MCMB graphite, carbon aerogels, carbon xerogel, carbon nano-fiber, nanotube, mesoporous carbon, Graphene.
Electrolyte solution of the present invention, its contained electrolytic salt is the solubility lithium salts, its amount of substance concentration is 0.1～5M; Contained solvent is non-proton organic solvent or ionic liquid.
Described solubility lithium salts is LiPF
6, LiN (CF
3SO
2)
2, LiBr, LiI, LiBF
4, (C
2H
5)
4NBF
4, LiCF
3SO
3, LiBC
4O
8, CH
3(C
2H
5)
3NBF
4Or LiClO
4, its amount of substance concentration is 0.1M～5M; Described non-proton organic solvent is propene carbonate, the rare fat of ethylene, glycol dimethyl ether or dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl propyl carbonate, 1,2-dimethoxy-ethane, gamma-butyrolacton, ethyl acetate.In 1, the 3-dioxolane one or two or more kinds.
When adopting 1M LiPF
6Propene carbonate is during as electrolyte solution, the category-A material with carbon element mainly contains Maxsorb 1470 (Kansai Coke and Chemicals), MCMB graphite (Osaka Gas Co.Ltd.), the category-B material with carbon element mainly contains Super P, Super S, Maxsorb 2400 (Kansai Coke and Chemicals), Maxsorb 3100 (Kansai Coke and Chemicals), C class material with carbon element mainly contains Denka Black, KB300, KB600, ENSACO 350G, Printex XE2, Printex XE2-B, HSAG300.
Also can contain catalyst in the described positive electrode, wherein the mass ratio of catalyst and material with carbon element is 4～0.01: 1, and more excellent scope is 1～0.05: 1.
Positive pole of the present invention, its preparation process is as follows:
1. will consist of the material with carbon element mechanical mixture of electrode material, mechanical mixture adopts known method, and for example ball milling perhaps stirs in solvent, sonic oscillation etc.
2. adopt known method, with mixing material with carbon element and binding agent that the first step obtains, such as PTFE, the mixing such as PVDF prepare positive pole.For example: will mix material with carbon element and PTFE with certain proportion in solvent, such as isopropyl alcohol, stir in ethanol or the water, sonic oscillation mixes, and obtains pasty mixture, adopts roll-in method to obtain the electrode pancake, strike out definite shape, colding pressing with nickel screen is integrated, and drying prepares electrode.
Prepared electrode and other battery component are assembled into lithium-air or lithium-oxygen monocell by known method, as adopt 2016 button cell shells as battery pack, successively with the lithium sheet, electrolyte membrance material (such as celgard 2340), electrode places on the battery cathode shell, drips electrolyte solution (such as 1M LiPF at electrode
6Carbonic allyl ester solution) some, to electrode and film complete wetting, rear electrodes anode cover (anode cover surface through hole is with transmission oxygen).On the button cell sealing machine, the said modules combined pressure is integrated, namely finishes the battery assembling.
Above-mentioned battery is placed dry pure oxygen environment (water content is lower than 1ppm), carry out the battery performance evaluation.
The present invention has the following advantages:
1. by in electrode, sneaking into lyophily material with carbon element or lyophobicity material with carbon element, guaranteeing that electrode is filled by electrolyte solution
Minute infiltrate when obtaining maximum solid-liquid two phase reaction interface, the material with carbon element stronger by lyophobicity makes up gas delivery passage, improved the mass transfer of oxygen at electrode, reduced it to the reaction interface diffusional resistance, increase the utilance of reaction interface, thereby improved the charge/discharge capacity of battery;
2. the material with carbon element of sneaking into improves electrode electrolyte inside Infiltrating and the oxygen transmission situation except playing, its
The place that itself also can carry out as electrode reaction simultaneously.
Description of drawings
The anodal electrochemical reaction model of Fig. 1;
Fig. 2 with KB600 and Super P complex carbon material (mass ratio 5: 1) with the discharge capacity of the cell contrast of KB600 as electrode material.
Embodiment:
Below by embodiment in detail the present invention is described in detail
Embodiment 1
Accurately take by weighing 100mg KB600 and 20mg Maxsorb 1470, stirring sonic oscillation in the 20ml isopropyl alcohol mixes the two, to wherein adding the 600mg 5wt.%PTFE aqueous solution, the stirring sonic oscillation mixes and obtains pasty mixture, with its repeatedly roll-in prepare the thick pancake shape electrode of 300 μ m, utilize mould to be made into the electrode of diameter 16mm, and cold pressing with nickel screen and to be integrated, obtain anode.
Adopt respectively simultaneously KB600 and Maxsorb 1470 material with carbon elements, prepare the control cell positive pole according to said process respectively.
As battery pack, successively with the lithium sheet, Celgard 2340 with 2016 button cell shells, and electrode places on the battery cathode shell, drip 1M LiPF at electrode
6The propene carbonate electrolyte solution is some, to electrode and film complete wetting, and rear electrodes anode cover (anode cover surface through hole is with transmission oxygen).On the button cell sealing machine, with said modules and consolidation, namely finish the battery assembling.
Be lower than in the pure oxygen environment of 1ppm at water content, for electrolyte solution, the electrode contact angle of KB600 and Maxsorb1470 preparation is respectively 42 ° and 119 °, and the combination electrode contact angle is 60 °.
Adopt the Arbin-BT2000 type to discharge and recharge instrument battery is carried out performance evaluation, the result shows that employing mixes material with carbon element type electrode, and the battery charging and discharging capacity relative improves 15% in KB600.
Embodiment 2
Accurately take by weighing 100mg Super P, 20mg KB300 and 10mg Maxsorb 1470, stirring sonic oscillation in the 20ml isopropyl alcohol mixes the three, to wherein adding the 650mg 5wt.%PTFE aqueous solution, stir sonic oscillation and mix and obtain pasty mixture, with its repeatedly roll-in prepare the thick pancake shape electrode of 300 μ m, utilize mould to be made into the electrode of diameter 16mm, and cold pressing with nickel screen and to be integrated, obtain anode.Adopt simultaneously Super P, KB300, Maxsorb 1470, prepare the control cell positive pole according to said process respectively.
As battery pack, successively with the lithium sheet, Celgard 2340 with 2016 button cell shells, and electrode places on the battery cathode shell, drip 1M LiPF at electrode
6The propene carbonate electrolyte solution is some, to electrode and film complete wetting, and rear electrodes anode cover (anode cover surface through hole is with transmission oxygen).On the button cell sealing machine, with said modules and consolidation, namely finish the battery assembling.
Be lower than in the pure oxygen environment of 1ppm at water content, for electrolyte solution, Super P, the electrode contact angle of KB300 and Maxsorb 1470 preparations is respectively 86.4 °, and 20.8 ° and 119 °, the combination electrode contact angle is 83 °.
Adopt the Arbin-BT2000 type to discharge and recharge instrument battery is carried out performance evaluation, the result shows that employing mixes material with carbon element type negative electrode, and the battery charging and discharging capacity relative improves 18% in Super P.
Embodiment 3
Accurately take by weighing 100mg Super P and 30mgKB300, stirring sonic oscillation in the 20ml isopropyl alcohol mixes the two, to wherein adding the 650mg 5wt.%PTFE aqueous solution, the stirring sonic oscillation mixes and obtains pasty mixture, with its repeatedly roll-in prepare the thick pancake shape electrode of 300 μ μ m, utilize mould to be made into the electrode of diameter 16mm, and cold pressing with nickel screen and to be integrated, obtain anode.Adopt simultaneously Super P, KB300 prepares the control cell positive pole according to said process respectively.
As battery pack, successively with the lithium sheet, Celgard 2340 with 2016 button cell shells, and electrode places on the battery cathode shell, drip 1M LiPF at electrode
6The propene carbonate electrolyte solution is some, to electrode and film complete wetting, and rear electrodes anode cover (anode cover surface through hole is with transmission oxygen).On the button cell sealing machine, with said modules and consolidation, namely finish the battery assembling.
Be lower than in the pure oxygen environment of 1ppm at water content, for electrolyte solution, Super P, the electrode contact angle of KB300 preparation is respectively 86.4 °, and 20.8 °, the combination electrode contact angle is 81 °.
Adopt the Arbin-BT2000 type to discharge and recharge instrument battery is carried out performance evaluation, the result shows that employing mixes material with carbon element type negative electrode, and the battery charging and discharging capacity relative improves 12% in Super P.
Embodiment 4
Accurately take by weighing 100mg KB600,20mg Super P, stirring sonic oscillation in the 20ml isopropyl alcohol mixes the three, to wherein adding the 600mg 5wt.%PTFE aqueous solution, stir sonic oscillation and mix and obtain pasty mixture, with its repeatedly roll-in prepare the thick pancake shape electrode of 300 μ m, utilize mould to be made into the electrode of diameter 16mm, and cold pressing with nickel screen and to be integrated, obtain anode.Adopt simultaneously KB600, Super P prepares the control cell positive pole according to said process respectively.
As battery pack, successively with the lithium sheet, Celgard 2340 with 2016 button cell shells, and electrode places on the battery cathode shell, drip 1M LiPF at electrode
6The rare ester of propene carbonate-ethylene (mass ratio is 2: 1) electrolyte solution is some, to electrode and film complete wetting, and rear electrodes anode cover (anode cover surface through hole is with transmission oxygen).On the button cell sealing machine, with said modules and consolidation, namely finish the battery assembling.
Be lower than in the pure oxygen environment of 1ppm at water content, for electrolyte solution, KB600, the electrode contact angle of SuperP preparation is respectively 52 ° and 96 °, and the combination electrode contact angle is 64 °.
Adopt the Arbin-BT2000 type to discharge and recharge instrument battery is carried out performance evaluation, the result shows that employing mixes material with carbon element type negative electrode, and the battery charging and discharging capacity relative improves 20% in KB600.
Embodiment 5
Accurately take by weighing 100mg KB600,10mg MCMB (Osaka Gas Co.Ltd), stirring sonic oscillation in the 20ml isopropyl alcohol mixes the three, to wherein adding the 550mg 5wt.%PTFE aqueous solution, stir sonic oscillation and mix and obtain pasty mixture, with its repeatedly roll-in prepare the thick pancake shape electrode of 300 μ m, utilize mould to be made into the electrode of diameter 16mm, and cold pressing with nickel screen and to be integrated, obtain anode.Adopt simultaneously KB600, MCMB (Osaka Gas Co.Ltd) prepares the control cell positive pole according to said process respectively.
As battery pack, successively with the lithium sheet, Celgard 2340 with 2016 button cell shells, and electrode places on the battery cathode shell, drip 1M LiPF at electrode
6The rare ester of propene carbonate-ethylene (mass ratio is 2: 1) electrolyte solution is some, to electrode and film complete wetting, and rear electrodes anode cover (anode cover surface through hole is with transmission oxygen).On the button cell sealing machine, with said modules and consolidation, namely finish the battery assembling.
Be lower than in the pure oxygen environment of 1ppm at water content, for electrolyte solution, KB600, the electrode contact angle of MCMB preparation is respectively 52 ° and 112 °, and the combination electrode contact angle is 68 °.
Adopt the Arbin-BT2000 type to discharge and recharge instrument battery is carried out performance evaluation, the result shows that employing mixes material with carbon element type negative electrode, and the battery charging and discharging capacity relative improves 20% in KB600.
Embodiment 6
Accurately take by weighing 100mg Super P, 15mg MCMB (Osaka Gas Co.Ltd), stirring sonic oscillation in the 20ml isopropyl alcohol mixes the three, to wherein adding the 575mg 5wt.%PTFE aqueous solution, stir sonic oscillation and mix and obtain pasty mixture, with its repeatedly roll-in prepare the thick pancake shape electrode of 300 μ m, utilize mould to be made into the electrode of diameter 16mm, and cold pressing with nickel screen and to be integrated, obtain anode.Adopt simultaneously Super P, MCMB (Osaka Gas Co.Ltd) prepares the control cell positive pole according to said process respectively.
As battery pack, successively with the lithium sheet, Celgard 2340 with 2016 button cell shells, and electrode places on the battery cathode shell, drip 1M LiPF at electrode
6Propene carbonate-glycol dimethyl ether (mass ratio is 1: 1) electrolyte solution is some, to electrode and film complete wetting, and rear electrodes anode cover (anode cover surface through hole is with transmission oxygen).On the button cell sealing machine, with said modules and consolidation, namely finish the battery assembling.
Be lower than in the pure oxygen environment of 1ppm at water content, for electrolyte solution, Super P, the electrode contact angle of MCMB preparation is respectively 49 ° and 108 °, and the combination electrode contact angle is 63 °.Adopt the Arbin-BT2000 type to discharge and recharge instrument battery is carried out performance evaluation, the result shows that employing mixes material with carbon element type negative electrode, and the battery charging and discharging capacity relative improves 10% in Super P.
Claims (5)
1. a lithium-air or lithium-aeration cell positive electrode is characterized in that: comprise two or three material with carbon element; Under the battery operation condition:
Material with carbon element A be to the electrolyte solution wettability relatively poor, and the contact angle of electrolyte solution between the 105-170 degree;
Material with carbon element B be the wettability to electrolyte solution moderate, and the contact angle of electrolyte solution between the 70-110 degree;
Material with carbon element C for electrolyte solution is had preferably infiltrating, and the contact angle of electrolyte solution between the 10-70 degree;
When comprising two kinds of material with carbon elements, positive electrode is A+B, wherein A: the B mass ratio is 0.05～10: 1; Or C+B, wherein C: the B mass ratio is 0.05～10: 1; Or A+C, wherein A: the C mass ratio is 0.05～20: 1;
When comprising three kinds of material with carbon elements, positive electrode is A+B+C, and wherein the mass fraction of B is 30-90%, A: the C mass ratio is 0.05～20: 1.
2. according to the described positive electrode of claim 1, it is characterized in that: the contained electrolytic salt of described electrolyte solution is the solubility lithium salts, and its amount of substance concentration is 0.1～5M; Contained solvent is non-proton organic solvent or ionic liquid.
3. according to the described positive electrode of claim 2, it is characterized in that: described solubility lithium salts is LiPF
6, LiN (CF
3SO
2)
2, LiBr, LiI, LiBF
4, (C
2H
5)
4NBF
4, LiCF
3SO
3, LiBC
4O
8, CH
3(C
2H
5)
3NBF
4Or LiClO
4Described non-proton organic solvent is propene carbonate, the rare fat of ethylene, glycol dimethyl ether or dimethyl carbonate, diethyl carbonate, methyl ethyl carbonate, methyl propyl carbonate, 1,2-dimethoxy-ethane, gamma-butyrolacton, ethyl acetate, 1, one or two or more kinds in the 3-dioxolane.
4. according to the described positive electrode of claim 1, it is characterized in that: described material with carbon element is nano-carbon material.
5. according to the described positive electrode of claim 1, it is characterized in that: also can contain catalyst in the described positive electrode, wherein the mass ratio of catalyst and material with carbon element is 4～0.01: 1, and more excellent scope is 1～0.05: 1.
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|---|---|---|---|
| CN201110314783.7A CN103050700B (en) | 2011-10-17 | 2011-10-17 | Positive electrode material for lithium-air battery or lithium-oxygen battery |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201110314783.7A CN103050700B (en) | 2011-10-17 | 2011-10-17 | Positive electrode material for lithium-air battery or lithium-oxygen battery |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114062201A (en) * | 2021-11-04 | 2022-02-18 | 湖北亿纬动力有限公司 | Method for detecting wettability of lithium ion battery electrolyte and application thereof |
| CN114447271A (en) * | 2021-12-30 | 2022-05-06 | 深圳市贝特瑞新能源技术研究院有限公司 | Preparation method of electrode plate, electrode plate and lithium ion battery |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102210042A (en) * | 2008-09-08 | 2011-10-05 | 新加坡南洋理工大学 | Electrode materials for metal-air batteries, fuel cells and supercapacitors |
-
2011
- 2011-10-17 CN CN201110314783.7A patent/CN103050700B/en active Active
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102210042A (en) * | 2008-09-08 | 2011-10-05 | 新加坡南洋理工大学 | Electrode materials for metal-air batteries, fuel cells and supercapacitors |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114062201A (en) * | 2021-11-04 | 2022-02-18 | 湖北亿纬动力有限公司 | Method for detecting wettability of lithium ion battery electrolyte and application thereof |
| CN114447271A (en) * | 2021-12-30 | 2022-05-06 | 深圳市贝特瑞新能源技术研究院有限公司 | Preparation method of electrode plate, electrode plate and lithium ion battery |
| CN114447271B (en) * | 2021-12-30 | 2024-04-26 | 深圳市贝特瑞新能源技术研究院有限公司 | Electrode slice preparation method, electrode slice and lithium ion battery |
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