CN103247823A - All-solid lithium-ion battery and manufacturing method thereof - Google Patents
All-solid lithium-ion battery and manufacturing method thereof Download PDFInfo
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- CN103247823A CN103247823A CN2013101395282A CN201310139528A CN103247823A CN 103247823 A CN103247823 A CN 103247823A CN 2013101395282 A CN2013101395282 A CN 2013101395282A CN 201310139528 A CN201310139528 A CN 201310139528A CN 103247823 A CN103247823 A CN 103247823A
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- 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 discloses an all-solid lithium-ion battery and a manufacturing method thereof. The all-solid lithium-ion battery comprises a positive pole material, a positive pole current collector, a solid electrolyte material, a negative pole material, a negative pole current collector and a stainless steel housing, wherein the solid electrolyte material is at least one selected from lanthanum lithium zirconate, strontium-doped lanthanum lithium zirconate, germanium-doped lanthanum lithium zirconate, aluminum-doped lanthanum lithium zirconate or silicon-doped lanthanum lithium zirconate. The manufacturing method of the battery is simple, and low in cost and energy consumption, and has a great application prospect in the future lithium-ion battery technology and market.
Description
Technical field
The present invention relates to electrochemical field, particularly, relate to a kind of all solid state lithium ion battery and preparation method thereof.
Background technology
Since the earlier 1990s commercialization, lithium ion battery in electric consumers, as fields such as mobile phone, notebook computer and digital cameras, has progressively occupied the increasing market share by feat of its high energy density and power density.Along with the continuous prosperity of national economy, with the continuous lifting of modern science and technology level, lithium ion battery has been expanded its application again greatly in current society.For reducing the electric automobile that CO2 emission is risen, and follow electronics miniaturization, the integrated and hull cell that produces etc. as in recent years.Its application has been expanded in the improvement of lithium-ion electric pool technology and perfect, again lithium ion battery has been proposed more harsh and high-end requirement with stylish service condition; Both influence each other and promote, have driven the common progress of scientific research and industrial economy.
At present, the commercial li-ion battery on the market is extensive use of liquid electrolyte, and it is inflammable and explosive organic substance, has take place to leak and temperature potential safety hazard such as blast when too high, can cause bigger personal injury and economic loss.Simultaneously, for some extreme environment, as highly integrated small-sized electronic product and high energy, stable energy-accumulating power station etc., existing lithium-ion electric pool technology all has been subjected to stern challenge.The lithium battery security incident occurs repeatedly, and lithium battery electrical automobile firing accident also makes the Arrested Development of present commercial dynamic lithium battery.
Therefore, the exploitation to lithium ion battery awaits further exploitation.
Summary of the invention
The present invention one of is intended to solve the problems of the technologies described above at least to a certain extent or provides a kind of useful commerce to select at least.For this reason, one object of the present invention is to propose a kind of all solid state lithium ion battery.This all solid state lithium ion battery has good thermal stability, chemical stability and machining property, thereby can fundamentally stop leakage, blast, make security performance obtain basic guarantee.
First aspect according to the embodiment of the invention, the invention provides a kind of all solid state lithium ion battery, comprise: positive electrode, plus plate current-collecting body, solid electrolyte material, negative material, negative current collector and stainless steel casing, wherein, described solid electrolyte material is at least a in lithium zirconate lanthanum, strontium doping lithium zirconate lanthanum, Ge-doped lithium zirconate lanthanum, aluminium doping lithium zirconate lanthanum or the silicon doping lithium zirconate lanthanum.Because the lithium zirconate lanthanum has a cube garnet structure, its by feat of higher conductivity at room temperature (as 10
-4S/cm) and electrochemical stability (as not reacting with lithium metal) can optimize and improve electrode and contact with interface between the electrolyte, be expected to promote the performance performance of all solid state lithium ion battery, have great application prospect.
According to the second aspect of the embodiment of the invention, the invention provides a kind of manufacture method of above-mentioned all solid state lithium ion battery, may further comprise the steps: solid electrolyte material is carried out surface finish handle; Positive active material and negative electrode active material are coated in the described two sides of passing through the solid electrolyte material of surface finish processing respectively; Outer surface at described positive active material and described negative electrode active material adds plus plate current-collecting body and negative current collector respectively, in order to obtain all solid state lithium ion battery structure; Encapsulate described all solid state lithium ion battery structure with stainless steel casing.The all solid state lithium ion battery that obtains by manufacture method provided by the invention, improved the fail safe of lithium battery greatly, simultaneously with respect to commercial batteries, have advantages such as operating process is easy, cost is low, energy consumption is little, in the lithium battery technology in future and market, have great application prospect.
Additional aspect of the present invention and advantage part in the following description provide, and part will become obviously from the following description, or recognize by practice of the present invention.
Description of drawings
Above-mentioned and/or additional aspect of the present invention and advantage are from obviously and easily understanding becoming the description of embodiment in conjunction with following accompanying drawing, wherein:
Fig. 1 is the structural representation according to all solid state lithium ion battery of the embodiment of the invention;
Fig. 2 is the charging and discharging curve according to all solid state lithium ion battery of the embodiment of the invention, LiMn2O4 just very wherein, and electrolyte is Ge-doped lithium zirconate lanthanum, and negative pole is lithium metal, and the charging/discharging voltage scope is 2.3V～4.6V.
Embodiment
Describe embodiments of the invention below in detail, the example of described embodiment is shown in the drawings, and wherein identical or similar label is represented identical or similar elements or the element with identical or similar functions from start to finish.Be exemplary below by the embodiment that is described with reference to the drawings, be intended to for explaining the present invention, and can not be interpreted as limitation of the present invention.
According to the first aspect of the embodiment of the invention, the invention provides a kind of all solid state lithium ion battery, comprising: positive electrode, plus plate current-collecting body, solid electrolyte material, negative material, negative current collector and stainless steel casing.According to embodiments of the invention, this solid electrolyte material is at least a in lithium zirconate lanthanum, strontium doping lithium zirconate lanthanum, Ge-doped lithium zirconate lanthanum, aluminium doping lithium zirconate lanthanum or the silicon doping lithium zirconate lanthanum.Because the lithium zirconate lanthanum has a cube garnet structure, its by feat of higher conductivity at room temperature (as 10
-4S/cm) and electrochemical stability (as not reacting with lithium metal) can optimize and improve electrode and contact with interface between the electrolyte, be expected to promote the performance performance of all solid state lithium ion battery, have great application prospect.
According to a particular embodiment of the invention, this all solid state lithium ion battery has layer structure.Thus, can further improve this all solid state lithium ion battery conductive performance and electrochemical stability, and security performance.
According to a particular embodiment of the invention, positive electrode is according to x:(100-x-y by positive active material, binding agent and conductive agent): y(is x 〉=70 wherein, y 〉=5) ratio preparation have a mobile slurry.According to embodiments of the invention, this active material is at least a in cobalt acid lithium, LiMn2O4, nickel-cobalt-manganese ternary material or the LiFePO4, and preferably, this positive active material is LiMn2O4.According to embodiments of the invention, this binding agent is at least a of Kynoar solution, polytetrafluoroethylsolution solution and poly-vinyl alcohol solution, and preferably, this binding agent is Kynoar solution.According to embodiments of the invention, described conductive agent is at least a in Super P, acetylene black and the graphite powder, and preferably, described conductive agent is Super P.According to embodiments of the invention, the ratio of this positive active material is not less than 70%, and the ratio of described conductive agent is not less than 5%.Thus, can further improve this all solid state lithium ion battery conductive performance and electrochemical stability, and security performance.
According to embodiments of the invention, this negative material is according to x:(100-x-y by negative electrode active material, binding agent and conductive agent): y(is x 〉=70 wherein, y 〉=5) slurry of ratio preparation.According to embodiments of the invention, this negative electrode active material is at least a in lithium metal, graphite, silicon or the lithium titanate, and preferably, described negative material is lithium metal.According to embodiments of the invention, this binding agent is at least a of Kynoar solution, polytetrafluoroethylsolution solution and poly-vinyl alcohol solution, and preferably, described binding agent is Kynoar solution.According to embodiments of the invention, this conductive agent is at least a in Super P, acetylene black and the graphite powder, and preferably, described conductive agent is Super P.According to embodiments of the invention, the ratio of this negative electrode active material is not less than 70%, and the ratio of described conductive agent is not less than 5%.Thus, can further improve this all solid state lithium ion battery conductive performance and electrochemical stability, and security performance.
According to a particular embodiment of the invention, described plus plate current-collecting body is at least a in stainless steel, copper or the aluminium, and preferably, described plus plate current-collecting body is aluminium.According to a particular embodiment of the invention, described negative current collector is at least a in stainless steel copper or the aluminium, and preferably, described negative current collector is copper.Thus, can further improve this all solid state lithium ion battery conductive performance and electrochemical stability, and security performance.
According to the second aspect of the embodiment of the invention, the invention provides a kind of manufacture method of above-mentioned all solid state lithium ion battery, may further comprise the steps: solid electrolyte material is carried out surface finish handle; Positive active material and negative electrode active material are coated in the described two sides of passing through the solid electrolyte material of surface finish processing respectively; Outer surface at described positive active material and described negative electrode active material adds plus plate current-collecting body and negative current collector respectively, in order to obtain all solid state lithium ion battery structure; Encapsulate described all solid state lithium ion battery structure with stainless steel casing.Thus, can obtain that electric conductivity is good, electrochemical stability good, all solid state lithium ion battery that security performance is high.
According to embodiments of the invention, the mode of the surface of solid electrolyte material being carried out polishing is not particularly limited.For example can polish with 200#～2000# sand paper according to an example of the present invention.Can obtain the surface of the solid electrolyte material of surfacing light thus.Thus, can obtain that electric conductivity is good, electrochemical stability good, all solid state lithium ion battery that security performance is high.
According to embodiments of the invention, positive active material and negative electrode active material are coated in respectively the described solid electrolyte material of handling through surface finish the two sides mode and be not particularly limited.For example according to a particular embodiment of the invention, can have the positive pole of mobile slurry form and the surface that negative material is coated in solid electrolyte with being configured to.According to a particular embodiment of the invention, when negative material is selected lithium metal for use, can directly be assembled to the surface of solid electrolyte.Can obtain having excellent conducting performance and electrochemical stability thus, and the high all solid state lithium ion battery of security performance.
According to embodiments of the invention, encapsulate described all solid state lithium ion battery structure with stainless steel casing, need there be metal terminal to be connected with plus plate current-collecting body, negative current collector respectively, so that carry out the charge and discharge process of battery.Can obtain having excellent conducting performance and electrochemical stability thus, and the high all solid state lithium ion battery of security performance.
According to a particular embodiment of the invention, described all solid state lithium ion battery is button cell or piece formula battery.The all solid state lithium ion battery that obtains by manufacture method provided by the invention, improved the fail safe of lithium battery greatly, simultaneously with respect to commercial batteries, have advantages such as operating process is easy, cost is low, energy consumption is little, in the lithium battery technology in future and market, have great application prospect.
Embodiment 1, making lithium manganate cathode all solid state lithium ion battery
Adopt LiMn2O4 as positive electrode, Ge-doped lithium zirconate lanthanum is as solid electrolyte, and lithium metal is as negative material, the assembling solid lithium ion battery.At first, extremely smooth at 300#, 800# and the polishing of 1500# sand paper successively for Ge-doped lithium zirconate lanthanum, ultrasonic processing is 10 minutes in ethanol, and 70 ℃ of oven dry, obtains the solid electrolyte of surface cleaning.LiMn2O4, PVDF and Super P are mixed according to the ratio of 80:5:15, be coated on the surface of solid electrolyte.Metal lithium sheet is attached to another surface of solid electrolyte.At last, add that at side of the positive electrode and negative side aluminium foil and Copper Foil are as collector respectively.Said structure is encapsulated in the stainless steel casing, finishes the making of all solid state lithium ion battery.
This all solid state lithium ion battery carries out charge-discharge test in the voltage range of 2.3V～4.6V, but stable circulation 100 times, its first charge-discharge curve as shown in Figure 2, discharge capacity can reach 98mAh/g first.
Embodiment 2, making lithium cobaltate cathode all solid state lithium ion battery
Adopt cobalt acid lithium as positive electrode, the lithium zirconate lanthanum that aluminium mixes is as solid electrolyte, and graphite is as negative material, the assembling solid lithium ion battery.At first, the lithium zirconate lanthanum that mixes for aluminium is extremely smooth at 500#, 1000# and the polishing of 2000# sand paper successively, and ultrasonic processing is 12 minutes in ethanol, and 90 ℃ of oven dry, obtains the solid electrolyte of surface cleaning.Cobalt acid lithium, PVA and the acetylene black ratio according to 90:5:5 is mixed, be coated on the surface of solid electrolyte.Graphite and PVA are mixed according to the ratio of 95:5, be coated on another surface of solid electrolyte.At last, add that at side of the positive electrode and negative side aluminium foil and Copper Foil are as collector respectively.Said structure is encapsulated in the stainless steel casing, finishes the making of all solid state lithium ion battery.
This all solid state lithium ion battery carries out charge-discharge test in the voltage range of 3.0～4.3V, but stable circulation 10 times, and discharge capacity can reach 74.4mAh/g first.
Embodiment 3, the anodal all solid state lithium ion battery of making nickel-cobalt-manganese ternary
Adopt the nickel-cobalt-manganese ternary material as positive electrode, Ge-doped lithium zirconate lanthanum is as solid electrolyte, and graphite is as negative material, the assembling solid lithium ion battery.At first, extremely smooth at 400#, 800# and the polishing of 1500# sand paper successively for Ge-doped lithium zirconate lanthanum, ultrasonic processing is 15 minutes in ethanol, and 80 ℃ of oven dry, obtains the solid electrolyte of surface cleaning.Nickel-cobalt-manganese ternary material, PVDF and Super P are mixed according to the ratio of 85:5:10, be coated on the surface of solid electrolyte.Graphite, conductive carbon black and PVDF are mixed according to the ratio of 90:5:5, be coated on another surface of solid electrolyte.At last, add that at side of the positive electrode and negative side aluminium foil and Copper Foil are as collector respectively.Said structure is encapsulated in the stainless steel casing, finishes the making of all solid state lithium ion battery.
This all solid state lithium ion battery carries out charge-discharge test in the voltage range of 3.0V～4.2V, but stable circulation 15 times, and discharge capacity can reach 94.4mAh/g first.
Embodiment 4, making iron phosphate lithium positive pole all solid state lithium ion battery
Adopt LiFePO4 as positive electrode, the lithium zirconate lanthanum of strontium doping is as solid electrolyte, and graphite is as negative material, the assembling solid lithium ion battery.At first, extremely smooth at 400#, 800# and the polishing of 1500# sand paper successively for the lithium zirconate lanthanum of strontium doping, ultrasonic processing is 12 minutes in ethanol, and 80 ℃ of oven dry, obtains the solid electrolyte of surface cleaning.LiFePO4, PVDF and Super P are mixed according to the ratio of 80:5:15, be coated on the surface of solid electrolyte.Graphite, conductive carbon black and PVDF are mixed according to the ratio of 88:5:7, be coated on another surface of solid electrolyte.At last, add that at side of the positive electrode and negative side aluminium foil and Copper Foil are as collector respectively.Said structure is encapsulated in the stainless steel casing, finishes the making of all solid state lithium ion battery.
This all solid state lithium ion battery carries out charge-discharge test in the voltage range of 2.2V～3.65V, but stable circulation 10 times, and discharge capacity can reach 120.3mAh/g first.
In the description of this specification, concrete feature, structure, material or characteristics that the description of reference term " embodiment ", " some embodiment ", " example ", " concrete example " or " some examples " etc. means in conjunction with this embodiment or example description are contained at least one embodiment of the present invention or the example.In this manual, the schematic statement to above-mentioned term not necessarily refers to identical embodiment or example.And concrete feature, structure, material or the characteristics of description can be with the suitable manner combination in any one or more embodiment or example.
Although illustrated and described embodiments of the invention above, be understandable that, above-described embodiment is exemplary, can not be interpreted as limitation of the present invention, those of ordinary skill in the art can change above-described embodiment under the situation that does not break away from principle of the present invention and aim within the scope of the invention, modification, replacement and modification.
Claims (8)
1. an all solid state lithium ion battery is characterized in that, comprising: positive electrode, plus plate current-collecting body, solid electrolyte material, negative material, negative current collector and stainless steel casing,
Wherein, described solid electrolyte material is at least a in lithium zirconate lanthanum, strontium doping lithium zirconate lanthanum, Ge-doped lithium zirconate lanthanum, aluminium doping lithium zirconate lanthanum or the silicon doping lithium zirconate lanthanum.
2. all solid state lithium ion battery according to claim 1, wherein, described all solid state lithium ion battery has layer structure.
3. all solid state lithium ion battery according to claim 1, wherein, described positive electrode is the slurry by positive active material, binding agent and conductive agent preparation,
Wherein, described positive active material is at least a in cobalt acid lithium, LiMn2O4, nickel-cobalt-manganese ternary material or the LiFePO4, and preferably, described positive active material is LiMn2O4;
Described binding agent is at least a of Kynoar solution, polytetrafluoroethylsolution solution and poly-vinyl alcohol solution, and preferably, described binding agent is Kynoar solution;
Described conductive agent is at least a in Super P, acetylene black and the graphite powder, and preferably, described conductive agent is Super P;
The ratio of described positive active material is not less than 70%, and the ratio of described conductive agent is not less than 5%.
4. all solid state lithium ion battery according to claim 1, wherein, described negative material is the slurry by negative electrode active material, binding agent and conductive agent preparation,
Wherein, described negative electrode active material is at least a in lithium metal, graphite, silicon or the lithium titanate, and preferably, described negative material is lithium metal,
Described binding agent is at least a of Kynoar solution, polytetrafluoroethylsolution solution and poly-vinyl alcohol solution, and preferably, described binding agent is Kynoar solution;
Described conductive agent is at least a in Super P, acetylene black and the graphite powder, and preferably, described conductive agent is Super P;
The ratio of described negative electrode active material is not less than 70%, and the ratio of described conductive agent is not less than 5%.
5. all solid state lithium ion battery according to claim 1, wherein, described plus plate current-collecting body is at least a in stainless steel, copper or the aluminium, preferably, described plus plate current-collecting body is aluminium.
6. all solid state lithium ion battery according to claim 1, wherein, described negative current collector is at least a in stainless steel copper or the aluminium, preferably, described negative current collector is copper.
7. the manufacture method as each described all solid state lithium ion battery of claim 1～6 is characterized in that, may further comprise the steps:
Solid electrolyte material is carried out surface finish to be handled;
Positive active material and negative electrode active material are coated in the described two sides of passing through the solid electrolyte material of surface finish processing respectively;
Outer surface at described positive active material and described negative electrode active material adds plus plate current-collecting body and negative current collector respectively, in order to obtain all solid state lithium ion battery structure;
Encapsulate described all solid state lithium ion battery structure with stainless steel casing.
8. the manufacture method of all solid state lithium ion battery according to claim 7, wherein, described all solid state lithium ion battery is button cell or piece formula battery.
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| CN105977527A (en) * | 2015-03-10 | 2016-09-28 | Tdk株式会社 | Garnet-type Li-ion conductive oxide |
| CN106159314A (en) * | 2015-04-15 | 2016-11-23 | 微宏动力系统（湖州）有限公司 | All-solid lithium-ion battery and preparation method thereof |
| CN108365259A (en) * | 2018-02-08 | 2018-08-03 | 南京大学 | A kind of lithium ion solid electrolyte and the preparation method and application thereof |
| CN108574119A (en) * | 2018-05-22 | 2018-09-25 | 浙江锋锂新能源科技有限公司 | A kind of preparation method of all-solid-state battery integrated module |
| CN108598557A (en) * | 2018-05-22 | 2018-09-28 | 浙江锋锂新能源科技有限公司 | A kind of all-solid-state battery integrated module and the all-solid-state battery comprising the module |
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| CN111326717A (en) * | 2018-12-13 | 2020-06-23 | 深圳先进技术研究院 | Aluminum negative electrode material, preparation method and secondary battery |
| CN113675480A (en) * | 2021-07-19 | 2021-11-19 | 华南理工大学 | Lithium ion battery cell with sandwich structure, electric pile and preparation method thereof |
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Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN105977527A (en) * | 2015-03-10 | 2016-09-28 | Tdk株式会社 | Garnet-type Li-ion conductive oxide |
| CN105977527B (en) * | 2015-03-10 | 2019-03-15 | Tdk株式会社 | Carbuncle type lithium-ion-conducting oxide |
| CN106159314A (en) * | 2015-04-15 | 2016-11-23 | 微宏动力系统（湖州）有限公司 | All-solid lithium-ion battery and preparation method thereof |
| CN106159314B (en) * | 2015-04-15 | 2019-05-24 | 微宏动力系统（湖州）有限公司 | All-solid lithium-ion battery and preparation method thereof |
| CN108365259A (en) * | 2018-02-08 | 2018-08-03 | 南京大学 | A kind of lithium ion solid electrolyte and the preparation method and application thereof |
| CN108365259B (en) * | 2018-02-08 | 2020-10-27 | 南京大学 | Lithium ion solid electrolyte and preparation method and application thereof |
| CN108574119A (en) * | 2018-05-22 | 2018-09-25 | 浙江锋锂新能源科技有限公司 | A kind of preparation method of all-solid-state battery integrated module |
| CN108598557A (en) * | 2018-05-22 | 2018-09-28 | 浙江锋锂新能源科技有限公司 | A kind of all-solid-state battery integrated module and the all-solid-state battery comprising the module |
| CN111326717A (en) * | 2018-12-13 | 2020-06-23 | 深圳先进技术研究院 | Aluminum negative electrode material, preparation method and secondary battery |
| CN109687032A (en) * | 2018-12-28 | 2019-04-26 | 上海纳米技术及应用国家工程研究中心有限公司 | A kind of design method of lithium ion battery structure |
| CN113675480A (en) * | 2021-07-19 | 2021-11-19 | 华南理工大学 | Lithium ion battery cell with sandwich structure, electric pile and preparation method thereof |
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| CN103247823B (en) | 2016-02-24 |
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