CN105514492A - 一种锂离子电池用电解液 - Google Patents
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- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 26
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 25
- 239000003792 electrolyte Substances 0.000 title claims abstract description 18
- -1 phosphoryl imide salts Chemical class 0.000 claims abstract description 18
- HVLLSGMXQDNUAL-UHFFFAOYSA-N triphenyl phosphite Chemical compound C=1C=CC=CC=1OP(OC=1C=CC=CC=1)OC1=CC=CC=C1 HVLLSGMXQDNUAL-UHFFFAOYSA-N 0.000 claims abstract description 12
- 229910052731 fluorine Inorganic materials 0.000 claims abstract description 9
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 8
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 8
- FFUAGWLWBBFQJT-UHFFFAOYSA-N hexamethyldisilazane Chemical compound C[Si](C)(C)N[Si](C)(C)C FFUAGWLWBBFQJT-UHFFFAOYSA-N 0.000 claims abstract description 7
- 239000000654 additive Substances 0.000 claims abstract description 6
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 claims abstract description 5
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 5
- 229910052801 chlorine Inorganic materials 0.000 claims abstract description 5
- 239000003063 flame retardant Substances 0.000 claims abstract description 5
- 239000011737 fluorine Substances 0.000 claims abstract description 5
- 150000001875 compounds Chemical class 0.000 claims abstract description 3
- 150000003839 salts Chemical class 0.000 claims description 9
- 239000000203 mixture Substances 0.000 claims description 7
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- 230000000996 additive effect Effects 0.000 claims description 5
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical group O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 claims description 4
- 229910052744 lithium Inorganic materials 0.000 claims description 4
- STCOOQWBFONSKY-UHFFFAOYSA-N tributyl phosphate Chemical compound CCCCOP(=O)(OCCCC)OCCCC STCOOQWBFONSKY-UHFFFAOYSA-N 0.000 claims description 4
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- XZZNDPSIHUTMOC-UHFFFAOYSA-N triphenyl phosphate Chemical compound C=1C=CC=CC=1OP(OC=1C=CC=CC=1)(=O)OC1=CC=CC=C1 XZZNDPSIHUTMOC-UHFFFAOYSA-N 0.000 claims description 4
- 239000001273 butane Substances 0.000 claims description 3
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 claims description 3
- WVLBCYQITXONBZ-UHFFFAOYSA-N trimethyl phosphate Chemical compound COP(=O)(OC)OC WVLBCYQITXONBZ-UHFFFAOYSA-N 0.000 claims description 3
- FSSPGSAQUIYDCN-UHFFFAOYSA-N 1,3-Propane sultone Chemical compound O=S1(=O)CCCO1 FSSPGSAQUIYDCN-UHFFFAOYSA-N 0.000 claims description 2
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 claims description 2
- ZSTLPJLUQNQBDQ-UHFFFAOYSA-N azanylidyne(dihydroxy)-$l^{5}-phosphane Chemical compound OP(O)#N ZSTLPJLUQNQBDQ-UHFFFAOYSA-N 0.000 claims description 2
- 229940125773 compound 10 Drugs 0.000 claims description 2
- ZLVXBBHTMQJRSX-VMGNSXQWSA-N jdtic Chemical compound C1([C@]2(C)CCN(C[C@@H]2C)C[C@H](C(C)C)NC(=O)[C@@H]2NCC3=CC(O)=CC=C3C2)=CC=CC(O)=C1 ZLVXBBHTMQJRSX-VMGNSXQWSA-N 0.000 claims description 2
- 125000001424 substituent group Chemical group 0.000 claims description 2
- 229910013872 LiPF Inorganic materials 0.000 abstract description 2
- 101150058243 Lipf gene Proteins 0.000 abstract description 2
- 230000007797 corrosion Effects 0.000 abstract description 2
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- 125000000472 sulfonyl group Chemical group *S(*)(=O)=O 0.000 abstract 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 abstract 1
- 229910001290 LiPF6 Inorganic materials 0.000 abstract 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 abstract 1
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- 239000002001 electrolyte material Substances 0.000 abstract 1
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- 238000012360 testing method Methods 0.000 description 6
- 239000008151 electrolyte solution Substances 0.000 description 4
- 239000002002 slurry Substances 0.000 description 4
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 3
- 229910052799 carbon Inorganic materials 0.000 description 3
- 238000007599 discharging Methods 0.000 description 3
- 238000011056 performance test Methods 0.000 description 3
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- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 2
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- 239000003960 organic solvent Substances 0.000 description 2
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- QGHDLJAZIIFENW-UHFFFAOYSA-N 4-[1,1,1,3,3,3-hexafluoro-2-(4-hydroxy-3-prop-2-enylphenyl)propan-2-yl]-2-prop-2-enylphenol Chemical group C1=C(CC=C)C(O)=CC=C1C(C(F)(F)F)(C(F)(F)F)C1=CC=C(O)C(CC=C)=C1 QGHDLJAZIIFENW-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical class O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 1
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- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
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- 238000002360 preparation method Methods 0.000 description 1
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
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- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
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Abstract
本发明公开了一种锂离子电池用电解液，按照质量份数，其组成为：结构式(Ⅰ)表示的化合物10–20份、其他锂盐5–12份、含氟磺酰/磷酰亚胺盐或含氯磺酰/磷酰亚胺盐3-10份、4-氟-1，3-二氧戊环-2-酮70–80份、SEI成膜剂2-3份、抗过冲添加剂3-5份、阻燃剂0.5–1.5份、六甲基二硅胺烷或亚磷酸三苯酯1-2份；该电解质材料与锂离子电池电极材料具有较好的相容性，较高的热稳定性，耐氧化还原能力强，无铝箔腐蚀性等特点。如在未使用任何非水电解液功能性添加剂的情况下，比使用现有LiPF6电解液制备的锂离子电池，具有更加优异高温循环和储存性能。
Description
技术领域
本发明属于新材料和电化学技术领域，具体涉及锂离子电池用电解液。
背景技术
锂离子电池以其比能量高、无污染、无记忆效应、寿命长而著称。近年来，锂离子电池备受重视，得到推广和应用。小到电子手表、手机，大到电动自行车、汽车，广受欢迎，甚至在军事航天等领域，锂离子电池也是越来越获得青睐。锂离子电池已经深刻影响人们的日常生活和工作。
随着对锂离子电池的需求增加，对锂离子电池的要求也越来越高。但是，基于本身的特点，锂离子电池存在着一些不足。如倍率性能不佳，即不能快速充放电，这对于汽车等动力领域是不可接受的。在电池充放电过程中，锂离子的移动场所包括电极、电极/电解液界面、电解液等。由于锂离子电池电解液采用的是非水有机溶剂，如碳酸酯类，溶质一般为六氟磷酸锂等无机锂盐，二者相容性不好，导致锂盐在有机溶剂中的溶解性并不好，造成电解液的电导率往往较小。这将直接导致参与迁移的锂离子较少，如果充放电电流较大，将引起严重的极化问题，造成电池容量下降。并且，随着温度降低，这一问题将进一步恶化。锂离子电池的倍率性能不高，导致锂离子电池不能快速充放电。
发明内容
本发明所要解决的技术问题是：提供一种相容性好、锂盐溶解性好的锂离子电池用非水电解液。
为解决上述技术问题，本发明所采用的技术方案为：一种锂离子电池用电解液，按照质量份数，其组成为：结构式(Ⅰ)表示的化合物10–20份、其他锂盐5–12份、含氟磺酰/磷酰亚胺盐或含氯磺酰/磷酰亚胺盐3-8份、4-氟-1，3-二氧戊环-2-酮(又称氟代碳酸乙烯酯)90–120份、SEI成膜剂4-8份、抗过冲添加剂3-5份、阻燃剂0.5–1.5份、六甲基二硅胺烷或亚磷酸三苯酯1-2份；
所述结构式(Ⅰ)表示的化合物为：
其中，Rf＝CF3O(CF2CF2)n、HCF2O(CF2CF2)n或ICF2O(CF2CF2)n，n为1～6的整数；
所述的含氟磺酰/磷酰亚胺盐或含氯磺酰/磷酰亚胺盐，分子式分别为：[(FSO2)(RfSO2)N]Li，[(F2PO)][(RfSO2)N]Li，[(ClSO2)(RfSO2)N]Li，[(Cl2PO)(RfSO2)N]Li；其结构通式为式(II)所示：
Rf＝CmF2m+1，m＝0－8，X＝SO2，Y＝Cl或F，n＝1；
或
Rf＝CmF2m+1，m＝0－8，X＝PO，Y＝Cl或F，n＝2；
所述其他锂盐为[N(SO2OCH2CF3)2]Li、N[SO2OCH(CF3)2]2Li、LiN(SO2RF)2、LiN(SO2F)(SO2RF)中的一种或二种以上的组合，其中取代基RF＝CnF2n+1，n为1至10的整数。
所述的SEI成膜剂为碳酸亚乙烯酯、氟代乙烯酯、氯代乙烯酯、丙烷磺酸内酯、氟代丙烷磺酸内酯、丁烷磺酸内酯、四烷基-二烯基硅氧烷、(对乙烯基苯磺酰)(全氟烷基磺酰)亚胺盐中的一种或二种以上的混合物。
所述阻燃剂为磷酸三甲酯(TMP)、磷酸三乙酯(TEP)、磷酸三苯酯(TPP)、磷酸三丁酯(TBP)、六甲基磷腈(HMPN)中的一种或二种以上的混合物。
本发明创新点在于：该电解质材料与锂离子电池电极材料具有较好的相容性，较高的热稳定性，耐氧化还原能力强，无铝箔腐蚀性等特点。如在未使用任何非水电解液功能性添加剂的情况下，比使用现有LiPF6电解液制备的锂离子电池，具有更加优异高温循环和储存性能。
具体实施方式
下面列举的具体实施例，是对本发明作进一步详细的说明，这些实施例仅用于说明本发明的目的，不以任何方式限制本发明所包含内容的范围。
实施例1
1)正极的制作：将LiCoO2粉末、炭黑(粒度为1000nm)、聚偏氟乙烯(PVDF)和N,N-二甲基吡咯烷酮(NMP)混合制成均一的浆料，将浆料均匀涂敷在铝箔(15μm)集流体上，然后进行干燥，轧制，得到LiCoO2正极材料。于120℃下烘12小时，干燥后的极片中，LiCoO2占总涂敷物的94％，粘结剂占4％，炭黑占2％。然后将所得极片裁剪成直径为12mm圆片作为正极。
2)负极的制作：将人造石墨，聚偏氟乙烯(PVDF)和N,N-二甲基吡咯烷酮(NMP)混合制成均一的浆料，将浆料均匀涂敷在铜箔(15μm)集流体上，然后进行干燥，轧制，得到碳负极材料。于120℃下烘12小时，干燥后的极片中，石墨占总涂敷物的96.4％，粘结剂占3.6％，然后将所得极片裁剪成直径为12mm圆片作为负极。
3)电解液的配制：
15份、[N(SO2OCH2CF3)2]Li8份、[(FSO2)(C2F5SO2)N]Li5份、4-氟-1，3-二氧戊环-2-酮98份、氟代乙烯酯5份、抗过冲添加剂4份、磷酸三乙酯0.8份、六甲基二硅胺烷或亚磷酸三苯酯1.5份；
将导电盐[N(SO2OCH2CF3)2]Li、[(FSO2)(C2F5SO2)N]Li真空干燥后转入手套箱，缓慢加入有机溶剂中，配制成电解液，密封待用。
4)CR2032扣式锂离子电池的组成及性能评价：将电池隔膜放在上述步骤1)和2)中所制备的正负极片之间，滴加上述步骤3)中所配制好的非水电解液，组装成CR2032的扣式电池。
在微机控制的自动充放仪(Land,CT2001A)上进行电池的循环性能测试。测试条件：温度为25℃，截止电压为4.2～2.75V，充电倍率为0.5C，放电倍率为0.2C。本实施例的测试数据参见表1。
实施例2
对比实施例1，18份、N[SO2OCH(CF3)2]2Li11份、[(ClSO2)(C3F7SO2)N]Li6份、4-氟-1，3-二氧戊环-2-酮110份、氟代丙烷磺酸内酯6份、抗过冲添加剂4份、磷酸三苯酯0.8份、六甲基二硅胺烷或亚磷酸三苯酯2份；
按实施例1中步骤1)～4)的操作，组装和评价电池。本实施例的测试数据参见表1。
实施例3
12份、LiN(SO2F)(SO2C2F5)11份、[(Cl2PO)(C2F5SO2)N]Li5份、4-氟-1，3-二氧戊环-2-酮120份、丁烷磺酸内酯2份、四烷基-二烯基硅氧烷3份、抗过冲添加剂3-5份、磷酸三苯酯0.6、磷酸三丁酯0.7份、六甲基二硅胺烷或亚磷酸三苯酯2份；
组装成和实施例1一样的电池，进行高温循环性能测试。测试条件：组装好的电池直接在60℃的恒温实验箱进行高温循环测试，截止电压为4.2–2.75V。充电倍率为0.5C，放电倍率为0.2C。本实施例的测试数据参见表1。
实施例1–3的电解液组成和电池性能测试数据见表1。
表1.非水电解液的组成及其锂离子电池在高温60℃或85℃存储实验前后的电化学性能数据。
Claims (3)
1.一种锂离子电池用电解液，按照质量份数，其组成为：结构式(Ⅰ)表示的化合物10–20份、其他锂盐5–12份、含氟磺酰/磷酰亚胺盐或含氯磺酰/磷酰亚胺盐3-8份、4-氟-1，3-二氧戊环-2-酮90–120份、SEI成膜剂4-8份、抗过冲添加剂3-5份、阻燃剂0.5–1.5份、六甲基二硅胺烷或亚磷酸三苯酯1-2份；
所述结构式(Ⅰ)表示的化合物为：
其中，Rf＝CF3O(CF2CF2)n、HCF2O(CF2CF2)n或ICF2O(CF2CF2)n，n为1～6的整数；
所述的含氟磺酰/磷酰亚胺盐或含氯磺酰/磷酰亚胺盐，分子式分别为：[(FSO2)(RfSO2)N]Li，[(F2PO)][(RfSO2)N]Li，[(ClSO2)(RfSO2)N]Li，[(Cl2PO)(RfSO2)N]Li；其结构通式为式(II)所示：
Rf＝CmF2m+1，m＝0－8，X＝SO2，Y＝Cl或F，n＝1；
或
Rf＝CmF2m+1，m＝0－8，X＝PO，Y＝Cl或F，n＝2；
所述其他锂盐为[N(SO2OCH2CF3)2]Li、N[SO2OCH(CF3)2]2Li、LiN(SO2RF)2、LiN(SO2F)(SO2RF)中的一种或二种以上的组合，其中取代基RF＝CnF2n+1，n为1至10的整数。
2.根据权利要求1所述一种锂离子电池用电解液，其特征在于：所述的SEI成膜剂为碳酸亚乙烯酯、氟代乙烯酯、氯代乙烯酯、丙烷磺酸内酯、氟代丙烷磺酸内酯、丁烷磺酸内酯、四烷基-二烯基硅氧烷、(对乙烯基苯磺酰)(全氟烷基磺酰)亚胺盐中的一种或二种以上的混合物。
3.根据权利要求1所述一种锂离子电池用电解液，其特征在于：所述阻燃剂为磷酸三甲酯、磷酸三乙酯、磷酸三苯酯、磷酸三丁酯、六甲基磷腈中的一种或二种以上的混合物。
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