CN103247823B - All-solid lithium-ion battery and preparation method thereof - Google Patents
All-solid lithium-ion battery and preparation method thereof Download PDFInfo
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Abstract
The invention provides a kind of all-solid lithium-ion battery and preparation method thereof.This all-solid lithium-ion battery comprises: positive electrode, plus plate current-collecting body, solid electrolyte material, negative material, negative current collector and stainless steel casing, wherein, solid electrolyte material is at least one in lithium zirconate lanthanum, strontium doping lithium zirconate lanthanum, Ge-doped lithium zirconate lanthanum, aluminium doping lithium zirconate lanthanum or silicon doping lithium zirconate lanthanum.The manufacturing process of this battery is simple, and cost is low, it is little to consume energy, in the lithium battery technology and market in future, have great application prospect.
Description
Technical field
The present invention relates to electrochemical field, particularly, relate to a kind of all-solid lithium-ion battery and preparation method thereof.
Background technology
Since earlier 1990s commercialization, lithium ion battery, by feat of its higher energy density and power density, in electric consumers, as fields such as mobile phone, notebook computer and digital cameras, progressively occupies the increasing market share.Along with the continuous prosperity of national economy, with the continuous lifting of modern science and technology level, lithium ion battery extends its application again greatly at society.As in recent years for reducing CO2 emission and the electric automobile that rises, and with electronics miniaturization, the integrated and hull cell etc. that produces.The improvement and perfection of lithium ion battery technology, extends its application, proposes more harsh Yu high-end requirement again with stylish service condition to lithium ion battery; Both influence each other and promotion, have driven the common progress of scientific research and industrial economy.
At present, the commercial li-ion battery on market widely uses liquid electrolyte, and it is inflammable and explosive organic substance, have occur to leak and temperature is too high time the potential safety hazard such as blast, larger personal injury and economic loss can be caused.Meanwhile, for some extreme environment, as highly integrated small-sized electronic product and high energy, stable energy-accumulating power station etc., existing lithium ion battery technology all receives stern challenge.Lithium battery security incident occurs repeatedly, and lithium cell electric vehicle fire accident also makes the Arrested Development of current commercial dynamic lithium battery.
Therefore, further exploitation is awaited to the exploitation of lithium ion battery.
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 at least provides a kind of useful business to select.For this reason, one object of the present invention is to propose a kind of all-solid lithium-ion battery.This all-solid lithium-ion battery, has good thermal stability, chemical stability and machining property, thus can fundamentally stop leakage, blast, make security performance obtain basic guarantee.
According to the first aspect of the embodiment of the present invention, the invention provides a kind of all-solid 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 one in lithium zirconate lanthanum, strontium doping lithium zirconate lanthanum, Ge-doped lithium zirconate lanthanum, aluminium doping lithium zirconate lanthanum or silicon doping lithium zirconate lanthanum.Because lithium zirconate lanthanum has cubic garnet structure, its by feat of higher conductivity at room temperature (as 10
-4s/cm) and electrochemical stability (as lithium metal does not react) interracial contact improved between electrode and electrolyte can be optimized, be expected to promote the performance of all-solid lithium-ion battery, there is great application prospect.
According to the second aspect of the embodiment of the present invention, the invention provides a kind of manufacture method of above-mentioned all-solid lithium-ion battery, comprise the following steps: surface finish process is carried out to solid electrolyte material; Positive active material and negative electrode active material are coated in respectively the two sides of the described solid electrolyte material through surface finish process; Plus plate current-collecting body and negative current collector is added respectively, to obtain all-solid lithium-ion battery structure at the outer surface of described positive active material and described negative electrode active material; Described all-solid lithium-ion battery structure is encapsulated with stainless steel casing.By the all-solid lithium-ion battery that manufacture method provided by the invention obtains, substantially increase the fail safe of lithium battery, simultaneously relative to commercial batteries, there is the advantages such as operating process is easy, cost is low, energy consumption is little, in the lithium battery technology and market in future, there is great application prospect.
Additional aspect of the present invention and advantage will part provide in the following description, and part will become obvious from the following description, or be recognized by practice of the present invention.
Accompanying drawing explanation
Above-mentioned and/or additional aspect of the present invention and advantage will become obvious and easy understand from accompanying drawing below combining to the description of embodiment, wherein:
Fig. 1 is the structural representation of the all-solid lithium-ion battery according to the embodiment of the present invention;
Fig. 2 is the charging and discharging curve of the all-solid lithium-ion battery according to the embodiment of the present invention, wherein just very LiMn2O4, and electrolyte is Ge-doped lithium zirconate lanthanum, and negative pole is lithium metal, and charging/discharging voltage scope is 2.3V ~ 4.6V.
Embodiment
Be described below in detail embodiments of the invention, the example of described embodiment is shown in the drawings, and wherein same or similar label represents same or similar element or has element that is identical or similar functions from start to finish.Be exemplary below by the embodiment be described with reference to the drawings, be intended to for explaining the present invention, and can not limitation of the present invention be interpreted as.
According to the first aspect of the embodiment of the present invention, the invention provides a kind of all-solid 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 one in lithium zirconate lanthanum, strontium doping lithium zirconate lanthanum, Ge-doped lithium zirconate lanthanum, aluminium doping lithium zirconate lanthanum or silicon doping lithium zirconate lanthanum.Because lithium zirconate lanthanum has cubic garnet structure, its by feat of higher conductivity at room temperature (as 10
-4s/cm) and electrochemical stability (as lithium metal does not react) interracial contact improved between electrode and electrolyte can be optimized, be expected to promote the performance of all-solid lithium-ion battery, there is great application prospect.
According to a particular embodiment of the invention, this all-solid lithium-ion battery has layer structure.Thus, this all-solid lithium-ion battery electric conductivity and electrochemical stability can be improved further, 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) slurry with mobility of proportions.According to embodiments of the invention, this active material is at least one in cobalt acid lithium, LiMn2O4, nickel-cobalt-manganese ternary material or LiFePO4, and preferably, this positive active material is LiMn2O4.According to embodiments of the invention, this binding agent is at least one 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 one in SuperP, acetylene black and graphite powder, and preferably, described conductive agent is SuperP.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, this all-solid lithium-ion battery electric conductivity and electrochemical stability can be improved further, 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 proportions.According to embodiments of the invention, this negative electrode active material is at least one in lithium metal, graphite, silicon or lithium titanate, and preferably, described negative material is lithium metal.According to embodiments of the invention, this binding agent is at least one 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 one in SuperP, acetylene black and graphite powder, and preferably, described conductive agent is SuperP.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, this all-solid lithium-ion battery electric conductivity and electrochemical stability can be improved further, and security performance.
According to a particular embodiment of the invention, described plus plate current-collecting body is at least one in stainless steel, copper or 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 one in stainless steel copper or aluminium, and preferably, described negative current collector is copper.Thus, this all-solid lithium-ion battery electric conductivity and electrochemical stability can be improved further, and security performance.
According to the second aspect of the embodiment of the present invention, the invention provides a kind of manufacture method of above-mentioned all-solid lithium-ion battery, comprise the following steps: surface finish process is carried out to solid electrolyte material; Positive active material and negative electrode active material are coated in respectively the two sides of the described solid electrolyte material through surface finish process; Plus plate current-collecting body and negative current collector is added respectively, to obtain all-solid lithium-ion battery structure at the outer surface of described positive active material and described negative electrode active material; Described all-solid lithium-ion battery structure is encapsulated with stainless steel casing.Thus, can obtain that electric conductivity is good, electrochemical stability good, the all-solid 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 to polishing is not particularly limited.Such as according to an example of the present invention, can polish with 200# ~ 2000# sand paper.The surface of the solid electrolyte material of surfacing light can be obtained thus.Thus, can obtain that electric conductivity is good, electrochemical stability good, the all-solid lithium-ion battery that security performance is high.
According to embodiments of the invention, positive active material and negative electrode active material be coated in respectively the mode on the two sides of the described solid electrolyte material through surface finish process and be not particularly limited.Such as according to a particular embodiment of the invention, the positive pole and negative material that are configured to the slurry form with mobility can be coated in the surface of solid electrolyte.According to a particular embodiment of the invention, when negative material selects lithium metal, directly can be assembled to the surface of solid electrolyte.Can obtain that there is good electric conductivity and electrochemical stability thus, and the all-solid lithium-ion battery that security performance is high.
According to embodiments of the invention, encapsulate described all-solid lithium-ion battery structure with stainless steel casing, need metal terminal and 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 that there is good electric conductivity and electrochemical stability thus, and the all-solid lithium-ion battery that security performance is high.
According to a particular embodiment of the invention, described all-solid lithium-ion battery is button cell or block formula battery.By the all-solid lithium-ion battery that manufacture method provided by the invention obtains, substantially increase the fail safe of lithium battery, simultaneously relative to commercial batteries, there is the advantages such as operating process is easy, cost is low, energy consumption is little, in the lithium battery technology and market in future, there is great application prospect.
Embodiment 1, making lithium manganate cathode all-solid lithium-ion battery
Adopt LiMn2O4 as positive electrode, Ge-doped lithium zirconate lanthanum as solid electrolyte, lithium metal as negative material, assembling solid lithium ion battery.First, Ge-doped lithium zirconate lanthanum is polished successively to smooth on 300#, 800# and 1500# sand paper, ultrasonic process 10 minutes in ethanol, and 70 DEG C of oven dry, obtain the solid electrolyte of clean surface.LiMn2O4, PVDF and SuperP are mixed according to the ratio of 80:5:15, is coated on the surface of solid electrolyte.Metal lithium sheet is attached to another surface of solid electrolyte.Finally, add that aluminium foil and Copper Foil are as collector at side of the positive electrode and negative side respectively.Said structure is encapsulated in stainless steel casing, completes the making of all-solid lithium-ion battery.
This all-solid lithium-ion battery carries out charge-discharge test in the voltage range of 2.3V ~ 4.6V, and Absorbable organic halogens circulates 100 times, and as shown in Figure 2, discharge capacity can reach 98mAh/g to its first charge-discharge curve first.
Embodiment 2, making lithium cobaltate cathode all-solid lithium-ion battery
Adopt cobalt acid lithium as positive electrode, aluminium doping lithium zirconate lanthanum as solid electrolyte, graphite as negative material, assembling solid lithium ion battery.First, the lithium zirconate lanthanum for aluminium doping is polished successively to smooth on 500#, 1000# and 2000# sand paper, ultrasonic process 12 minutes in ethanol, and 90 DEG C of oven dry, obtains the solid electrolyte of clean surface.Cobalt acid lithium, PVA and acetylene black are mixed according to the ratio of 90:5:5, is coated on the surface of solid electrolyte.Graphite and PVA are mixed according to the ratio of 95:5, be coated to solid electrolyte another on the surface.Finally, add that aluminium foil and Copper Foil are as collector at side of the positive electrode and negative side respectively.Said structure is encapsulated in stainless steel casing, completes the making of all-solid lithium-ion battery.
This all-solid lithium-ion battery carries out charge-discharge test in the voltage range of 3.0 ~ 4.3V, and Absorbable organic halogens circulates 10 times, and discharge capacity can reach 74.4mAh/g first.
Embodiment 3, making nickel-cobalt-manganese ternary positive pole all-solid lithium-ion battery
Adopt nickel-cobalt-manganese ternary material as positive electrode, Ge-doped lithium zirconate lanthanum as solid electrolyte, graphite as negative material, assembling solid lithium ion battery.First, Ge-doped lithium zirconate lanthanum is polished successively to smooth on 400#, 800# and 1500# sand paper, ultrasonic process 15 minutes in ethanol, and 80 DEG C of oven dry, obtain the solid electrolyte of clean surface.Nickel-cobalt-manganese ternary material, PVDF and SuperP are mixed according to the ratio of 85:5:10, is 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 to solid electrolyte another on the surface.Finally, add that aluminium foil and Copper Foil are as collector at side of the positive electrode and negative side respectively.Said structure is encapsulated in stainless steel casing, completes the making of all-solid lithium-ion battery.
This all-solid lithium-ion battery carries out charge-discharge test in the voltage range of 3.0V ~ 4.2V, and Absorbable organic halogens circulates 15 times, and discharge capacity can reach 94.4mAh/g first.
Embodiment 4, making iron phosphate lithium positive pole all-solid lithium-ion battery
Adopt LiFePO4 as positive electrode, the lithium zirconate lanthanum of strontium doping as solid electrolyte, graphite as negative material, assembling solid lithium ion battery.First, the lithium zirconate lanthanum for strontium doping is polished successively to smooth on 400#, 800# and 1500# sand paper, ultrasonic process 12 minutes in ethanol, and 80 DEG C of oven dry, obtains the solid electrolyte of clean surface.LiFePO4, PVDF and SuperP are mixed according to the ratio of 80:5:15, is 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 to solid electrolyte another on the surface.Finally, add that aluminium foil and Copper Foil are as collector at side of the positive electrode and negative side respectively.Said structure is encapsulated in stainless steel casing, completes the making of all-solid lithium-ion battery.
This all-solid lithium-ion battery carries out charge-discharge test in the voltage range of 2.2V ~ 3.65V, and Absorbable organic halogens circulates 10 times, and discharge capacity can reach 120.3mAh/g first.
In the description of this specification, specific features, structure, material or feature that the description of reference term " embodiment ", " some embodiments ", " example ", " concrete example " or " some examples " etc. means to describe in conjunction with this embodiment or example are contained at least one embodiment of the present invention or example.In this manual, identical embodiment or example are not necessarily referred to the schematic representation of above-mentioned term.And the specific features of description, structure, material or feature can combine in an appropriate manner in any one or more embodiment or example.
Although illustrate and describe 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 within the scope of the invention when not departing from principle of the present invention and aim, revising, replacing and modification.
Claims (9)
1. a manufacture method for all-solid lithium-ion battery, is characterized in that, described all-solid lithium-ion battery comprises: 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 one in lithium zirconate lanthanum, strontium doping lithium zirconate lanthanum, Ge-doped lithium zirconate lanthanum, aluminium doping lithium zirconate lanthanum or silicon doping lithium zirconate lanthanum,
Described positive electrode is the slurry prepared by positive active material, binding agent and conductive agent,
Described positive active material is at least one in cobalt acid lithium, LiMn2O4, nickel-cobalt-manganese ternary material or LiFePO4;
Described binding agent is at least one of Kynoar solution, polytetrafluoroethylsolution solution and poly-vinyl alcohol solution;
Described conductive agent is SuperP;
The ratio of described positive active material is not less than 70%, and the ratio of described conductive agent is not less than 5%,
Described negative material is the slurry prepared by negative electrode active material, binding agent and conductive agent,
Described negative material is lithium metal,
Described binding agent is at least one of Kynoar solution, polytetrafluoroethylsolution solution and poly-vinyl alcohol solution;
Described conductive agent is SuperP;
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%,
Described negative material is the slurry prepared by negative electrode active material, binding agent and conductive agent,
The manufacture method of described all-solid lithium-ion battery comprises the following steps:
Surface finish process is carried out to solid electrolyte material;
Positive electrode and negative material are coated in respectively the two sides of the solid electrolyte material through surface finish process;
Plus plate current-collecting body and negative current collector is added respectively, to obtain all-solid lithium-ion battery structure at the outer surface of described positive electrode and described negative material;
Described all-solid lithium-ion battery structure is encapsulated with stainless steel casing.
2. the manufacture method of all-solid lithium-ion battery according to claim 1, wherein, described all-solid lithium-ion battery is button cell or block formula battery.
3. the manufacture method of all-solid lithium-ion battery according to claim 1, wherein, described all-solid lithium-ion battery has layer structure.
4. the manufacture method of all-solid lithium-ion battery according to claim 1, wherein, described plus plate current-collecting body is at least one in stainless steel, copper or aluminium.
5. the manufacture method of all-solid lithium-ion battery according to claim 4, wherein, described plus plate current-collecting body is aluminium.
6. the manufacture method of all-solid lithium-ion battery according to claim 1, wherein, described negative current collector is at least one in stainless steel copper or aluminium.
7. the manufacture method of all-solid lithium-ion battery according to claim 6, wherein, described negative current collector is copper.
8. the manufacture method of all-solid lithium-ion battery according to claim 1, wherein, described binding agent is Kynoar solution.
9. the manufacture method of all-solid lithium-ion battery according to claim 1, wherein, described positive active material is LiMn2O4.
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JP2016171068A (en) * | 2015-03-10 | 2016-09-23 | Tdk株式会社 | Garnet-type lithium ion conductive oxide |
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 |
CN108365259B (en) * | 2018-02-08 | 2020-10-27 | 南京大学 | Lithium ion solid electrolyte and preparation method and application thereof |
CN108598557B (en) * | 2018-05-22 | 2020-06-23 | 浙江锋锂新能源科技有限公司 | All-solid-state battery integrated module and all-solid-state battery comprising same |
CN108574119B (en) * | 2018-05-22 | 2020-06-23 | 浙江锋锂新能源科技有限公司 | Preparation method of all-solid-state battery integrated module |
CN111326717B (en) * | 2018-12-13 | 2021-11-16 | 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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