CN106935800A - 用于二次锂电池负极的保护层 - Google Patents
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- 229910052744 lithium Inorganic materials 0.000 title claims abstract description 75
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims abstract description 66
- 239000011241 protective layer Substances 0.000 title claims abstract description 21
- 229910052751 metal Inorganic materials 0.000 claims abstract description 8
- 239000002184 metal Substances 0.000 claims abstract description 8
- 239000000843 powder Substances 0.000 claims abstract description 6
- GLNWILHOFOBOFD-UHFFFAOYSA-N lithium sulfide Chemical class [Li+].[Li+].[S-2] GLNWILHOFOBOFD-UHFFFAOYSA-N 0.000 claims abstract description 5
- 239000002904 solvent Substances 0.000 claims description 16
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 claims description 7
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 claims description 6
- 229910045601 alloy Inorganic materials 0.000 claims description 6
- 239000000956 alloy Substances 0.000 claims description 6
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N dimethyl sulfoxide Natural products CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 claims description 6
- 150000002148 esters Chemical class 0.000 claims description 6
- 150000003457 sulfones Chemical class 0.000 claims description 6
- 238000005868 electrolysis reaction Methods 0.000 claims description 5
- 238000002360 preparation method Methods 0.000 claims description 5
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 claims description 4
- 239000003795 chemical substances by application Substances 0.000 claims description 4
- ZUHZGEOKBKGPSW-UHFFFAOYSA-N tetraglyme Chemical compound COCCOCCOCCOCCOC ZUHZGEOKBKGPSW-UHFFFAOYSA-N 0.000 claims description 4
- SBZXBUIDTXKZTM-UHFFFAOYSA-N diglyme Chemical compound COCCOCCOC SBZXBUIDTXKZTM-UHFFFAOYSA-N 0.000 claims description 3
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 2
- YBJCDTIWNDBNTM-UHFFFAOYSA-N 1-methylsulfonylethane Chemical compound CCS(C)(=O)=O YBJCDTIWNDBNTM-UHFFFAOYSA-N 0.000 claims description 2
- XFXPMWWXUTWYJX-UHFFFAOYSA-N Cyanide Chemical compound N#[C-] XFXPMWWXUTWYJX-UHFFFAOYSA-N 0.000 claims description 2
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 claims description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical group COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 claims description 2
- AOJJSUZBOXZQNB-TZSSRYMLSA-N Doxorubicin Chemical compound O([C@H]1C[C@@](O)(CC=2C(O)=C3C(=O)C=4C=CC=C(C=4C(=O)C3=C(O)C=21)OC)C(=O)CO)[C@H]1C[C@H](N)[C@H](O)[C@H](C)O1 AOJJSUZBOXZQNB-TZSSRYMLSA-N 0.000 claims description 2
- 229910002651 NO3 Inorganic materials 0.000 claims description 2
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims description 2
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 2
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical group COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 2
- 229920001021 polysulfide Polymers 0.000 claims description 2
- 239000005077 polysulfide Substances 0.000 claims description 2
- 150000008117 polysulfides Polymers 0.000 claims description 2
- IJDNQMDRQITEOD-UHFFFAOYSA-N sec-butylidene Natural products CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 claims description 2
- 238000004073 vulcanization Methods 0.000 claims description 2
- BDHFUVZGWQCTTF-UHFFFAOYSA-M sulfonate Chemical compound [O-]S(=O)=O BDHFUVZGWQCTTF-UHFFFAOYSA-M 0.000 claims 1
- 210000001787 dendrite Anatomy 0.000 abstract description 6
- 238000000034 method Methods 0.000 abstract description 6
- 239000010410 layer Substances 0.000 abstract description 4
- 229910000733 Li alloy Inorganic materials 0.000 abstract 2
- 239000001989 lithium alloy Substances 0.000 abstract 2
- 239000012530 fluid Substances 0.000 description 4
- 239000011888 foil Substances 0.000 description 4
- 210000004027 cell Anatomy 0.000 description 3
- 229910000521 B alloy Inorganic materials 0.000 description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 2
- PPTSBERGOGHCHC-UHFFFAOYSA-N boron lithium Chemical compound [Li].[B] PPTSBERGOGHCHC-UHFFFAOYSA-N 0.000 description 2
- 229910001416 lithium ion Inorganic materials 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- LSNNMFCWUKXFEE-UHFFFAOYSA-M Bisulfite Chemical compound OS([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-M 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- JDZCKJOXGCMJGS-UHFFFAOYSA-N [Li].[S] Chemical compound [Li].[S] JDZCKJOXGCMJGS-UHFFFAOYSA-N 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 238000005524 ceramic coating Methods 0.000 description 1
- 230000004087 circulation Effects 0.000 description 1
- 229920000547 conjugated polymer Polymers 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 125000001033 ether group Chemical group 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 229920006254 polymer film Polymers 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/134—Electrodes based on metals, Si or alloys
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0416—Methods of deposition of the material involving impregnation with a solution, dispersion, paste or dry powder
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0438—Processes of manufacture in general by electrochemical processing
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- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
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- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
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Abstract
本发明涉及一种用于二次锂电池负极的保护层，能在锂负极上方便有效地形成一层保护层，从而有效延长锂负极的循环寿命，实现锂二次电池的高能量密度。锂二次电池中的金属锂负极包括所有类型金属锂的负极，包括金属锂片、锂箔、锂粉、锂粒，包括含锂合金的负极，包括锂合金的片、箔、粉、粒。在锂负极上形成保护层的方法是通过将金属锂在一种特殊溶液中浸泡或者电解；其中所涉及的特殊溶液是一种含有多硫化锂的溶液。有效解决锂负极的锂枝晶问题、锂负极的安全问题和循环寿命问题，使锂二次电池的高能量密度得以实现。
Description
技术领域
本发明涉及一种用于二次锂电池负极的保护层。属于电化学领域。
背景技术
随着科技的进步，人们迫切需要一种高能量密度电池来适应各种电池的小型化、轻量化趋势，这时，锂离子电池就很难满足需要。由于石墨的理论比能量的限制，锂离子电池很难成为高能量密度电池。在理论上以金属锂为负极的电池可以成为更高能量密度的电池。金属锂的比容量高达3860mAh/g，而且锂电极的交换电流密度大，极化小，是最为理想的电极材料。但由于金属锂电极在充放电过程中将产生锂枝晶。当锂枝晶从极板脱落，会导致电池容量的损失，若锂枝晶逐渐生，则可能刺穿隔膜而导致电池内部短路，引发电池起火或爆炸。此问题最终导致锂二次电池在市场上尚未获得成功。
对于保护锂负极，文献中也提出许多种方案，包括用聚合物、陶瓷或玻璃等保护层来涂覆在锂负极上。美国专利USP5460905、USP5462566描述了一种方法，在电池中锂负极与电解质之间掺一个共轭聚合物膜，而USP5648187和USP 5961672描述了在电池中的锂负极和电解质之间夹一层导电的聚合物膜及其制备方法；美国专利USP5314765还描述了锂负极上覆盖一层陶瓷涂层。还有一些方法，在美国专利USP5387479、USP5487959、CN1297588A、CN1726608A、CN1894821A、CN1938895A、CN101313426A等中有所描述。
尽管提出了各种各样的在锂负极上形成保护层的方法，但目前仍未解决锂负极的锂枝晶问题。仍需要提出更为有效的解决方法，来解决锂负极的安全问题和循环寿命问题，从而使锂二次电池的高能量密度得以实现。
发明内容
本发明的目的是提供一种用于二次锂电池负极的保护层，在锂负极上方便有效地形成一层保护层。
本发明采用的技术方案，用于二次锂电池负极的保护层的制备方法步骤如下：
将金属锂负极置于保护溶液中进行静置、振动、摇动、搅动或电解处理，处理温度为-20～120℃，压力为0.1～10dtm，处理时间为0.1～5h。其中，进行电解处理时，电压为0～5V，电流0～10A；
锂负极保护层的制备在电池组装前或在电池组装后；
金属锂负极为金属锂片、锂箔、锂粉、锂粒或金属锂合金，金属锂合金为金属锂合金的片、箔、粉或粒。
保护溶液包括处理剂和溶液两部分，处理剂为二硫化锂、四硫化锂、六硫化锂或八硫化锂；溶剂为醚类溶剂、酯类溶剂、烃类溶剂或砜类溶剂，醚类溶剂为乙二醇二甲醚、二乙二醇二甲醚、四乙二醇二甲醚或1，3-二氧戊环；酯类溶剂为碳酸二甲酯、碳酸二乙酯、碳酸甲乙酯或碳酸亚乙烯撑酯；烃类溶剂为正丁烷、甲苯或二甲苯；砜类溶剂为二甲基亚砜、环丁砜或甲基乙基砜；
用于二次锂电池的锂负极保护层的成分为多硫化物、氧化物、氰化物、硫酸盐、磺酸盐、硝酸盐中的一种以上。
本发明的有益效果：有效解决锂负极的锂枝晶问题、锂负极的安全问题和循环寿命问题，使锂二次电池的高能量密度得以实现。
具体实施方式
实施例1
将金属锂箔静置于0.2mol/L的Li2S6/1，3-二氧戊环处理溶液中1h，取出后用1，3-二氧戊环纯溶剂冲洗去除金属锂箔表面多余的处理液，得到具有保护层的金属锂箔。
将具有保护层的金属锂箔应用于锂硫电池中，在100mA/g电流密度下，正极材料首次放电容量1550mAh/g，50次循环后放电比容量为1000mAh/g。
实施例2
将金属锂片置于0.50mol/L的Li2S4/碳酸甲乙酯处理液中，超声振动2h，取出后用乙二醇二甲醚纯溶剂冲洗去除金属锂片表面多余的处理液，得到具有保护层的金属锂片。
实施例3
将锂硼合金片夹于铜电极上，然后置于0.50mol/L的Li2S2/环丁砜处理液中，另在处理液中插入铂电极作为对电极，设定电流2mA、电压3V进行电解处理2h，，得到具有保护层的锂硼合金片。
Claims (1)
1.一种用于二次锂电池负极的保护层，其特征在于该保护层的制备方法步骤如下：
将金属锂负极置于保护溶液中进行静置、振动、摇动、搅动或电解处理，处理温度为-20～120℃，压力为0.1～10dtm，时间为0.1～5h；其中，进行电解处理时，电压为0～5V，电流0～10A；
锂负极保护层的制备在电池组装前或在电池组装后；
金属锂负极为金属锂片、锂箔、锂粉、锂粒或金属锂合金，金属锂合金为金属锂合金的片、箔、粉或粒；
保护溶液包括处理剂和溶液两部分，处理剂为二硫化锂、四硫化锂、六硫化锂或八硫化锂；溶剂包括醚类溶剂、酯类溶剂、烃类溶剂或砜类溶剂，醚类溶剂为乙二醇二甲醚、二乙二醇二甲醚、四乙二醇二甲醚或1，3-二氧戊环；酯类溶剂为碳酸二甲酯、碳酸二乙酯、碳酸甲乙酯或碳酸亚乙烯撑酯；烃类溶剂为正丁烷、甲苯或二甲苯；砜类溶剂为二甲基亚砜、环丁砜或甲基乙基砜；
用于二次锂电池的锂负极保护层的成分为多硫化物、氧化物、氰化物、硫酸盐、磺酸盐、硝酸盐中的一种以上。
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN109273664A (zh) * | 2018-09-13 | 2019-01-25 | 中国电子科技集团公司第十八研究所 | 一种超薄锂箔的电化学制备方法 |
| CN109461886A (zh) * | 2018-11-19 | 2019-03-12 | 江西迪比科股份有限公司 | 一种复合型金属锂负极材料及制备方法 |
| CN109786692A (zh) * | 2018-12-25 | 2019-05-21 | 中国电子科技集团公司第十八研究所 | 一种金属锂电极的表面氮化修饰方法及获得的金属锂负极和用途 |
| CN111952571A (zh) * | 2020-08-24 | 2020-11-17 | 上海空间电源研究所 | 用于高功率一次电池的锂/锂合金复合负极、制备方法及电池 |
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| CN111952571A (zh) * | 2020-08-24 | 2020-11-17 | 上海空间电源研究所 | 用于高功率一次电池的锂/锂合金复合负极、制备方法及电池 |
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