CN104078710A - 一种宽温区不燃的锂离子电池电解液 - Google Patents
一种宽温区不燃的锂离子电池电解液 Download PDFInfo
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 35
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 35
- 239000008151 electrolyte solution Substances 0.000 title abstract 7
- 239000004721 Polyphenylene oxide Substances 0.000 claims abstract description 21
- 229920000570 polyether Polymers 0.000 claims abstract description 21
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 14
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 14
- 239000002904 solvent Substances 0.000 claims abstract description 5
- 239000003792 electrolyte Substances 0.000 claims description 43
- -1 lithium bis (trifluoromethanesulfonate) imide Chemical class 0.000 claims description 10
- MCVFFRWZNYZUIJ-UHFFFAOYSA-M lithium;trifluoromethanesulfonate Chemical compound [Li+].[O-]S(=O)(=O)C(F)(F)F MCVFFRWZNYZUIJ-UHFFFAOYSA-M 0.000 claims description 9
- 125000000217 alkyl group Chemical group 0.000 claims description 8
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 claims description 8
- 150000007942 carboxylates Chemical group 0.000 claims description 8
- 229910052731 fluorine Inorganic materials 0.000 claims description 8
- 229910052801 chlorine Inorganic materials 0.000 claims description 6
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 5
- 150000005676 cyclic carbonates Chemical group 0.000 claims description 5
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 5
- 229910052744 lithium Inorganic materials 0.000 claims description 5
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims description 4
- 229910052794 bromium Inorganic materials 0.000 claims description 4
- 125000004122 cyclic group Chemical group 0.000 claims description 4
- 125000004185 ester group Chemical group 0.000 claims description 4
- 229910052739 hydrogen Inorganic materials 0.000 claims description 4
- 150000005685 straight-chain carbonates Chemical group 0.000 claims description 4
- 229910052717 sulfur Inorganic materials 0.000 claims description 4
- 239000011593 sulfur Substances 0.000 claims description 4
- 238000000034 method Methods 0.000 claims description 3
- RWKIJHIGANBMOF-UHFFFAOYSA-N [Li]C(S(=O)(=O)C(F)(F)F)(S(=O)(=O)C(F)(F)F)S(=O)(=O)C(F)(F)F Chemical compound [Li]C(S(=O)(=O)C(F)(F)F)(S(=O)(=O)C(F)(F)F)S(=O)(=O)C(F)(F)F RWKIJHIGANBMOF-UHFFFAOYSA-N 0.000 claims description 2
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 claims description 2
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 claims description 2
- 125000001449 isopropyl group Chemical group [H]C([H])([H])C([H])(*)C([H])([H])[H] 0.000 claims description 2
- QVXQYMZVJNYDNG-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)methylsulfonyl-trifluoromethane Chemical compound [Li+].FC(F)(F)S(=O)(=O)[C-](S(=O)(=O)C(F)(F)F)S(=O)(=O)C(F)(F)F QVXQYMZVJNYDNG-UHFFFAOYSA-N 0.000 claims description 2
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 claims description 2
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 claims description 2
- QSZMZKBZAYQGRS-UHFFFAOYSA-N lithium;bis(trifluoromethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)F QSZMZKBZAYQGRS-UHFFFAOYSA-N 0.000 claims 1
- 239000007788 liquid Substances 0.000 abstract description 4
- 239000003960 organic solvent Substances 0.000 abstract description 3
- 238000002844 melting Methods 0.000 abstract description 2
- 230000008018 melting Effects 0.000 abstract description 2
- 150000002148 esters Chemical class 0.000 abstract 1
- 239000000460 chlorine Substances 0.000 description 6
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 description 4
- 239000011737 fluorine Substances 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 125000001889 triflyl group Chemical group FC(F)(F)S(*)(=O)=O 0.000 description 3
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 2
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 2
- 239000007983 Tris buffer Substances 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 150000001450 anions Chemical class 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 230000005518 electrochemistry Effects 0.000 description 2
- 239000003063 flame retardant Substances 0.000 description 2
- IHLVCKWPAMTVTG-UHFFFAOYSA-N lithium;carbanide Chemical compound [Li+].[CH3-] IHLVCKWPAMTVTG-UHFFFAOYSA-N 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 1
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 1
- 229910000552 LiCF3SO3 Inorganic materials 0.000 description 1
- 229910013870 LiPF 6 Inorganic materials 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 239000013543 active substance Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 150000001768 cations Chemical class 0.000 description 1
- 150000005678 chain carbonates Chemical class 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000002360 explosive Substances 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- GELKBWJHTRAYNV-UHFFFAOYSA-K lithium iron phosphate Chemical group [Li+].[Fe+2].[O-]P([O-])([O-])=O GELKBWJHTRAYNV-UHFFFAOYSA-K 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 150000003013 phosphoric acid derivatives Chemical class 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 229910000029 sodium carbonate Inorganic materials 0.000 description 1
- 229920001059 synthetic polymer Polymers 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- 230000003313 weakening effect Effects 0.000 description 1
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- 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
- H01M10/056—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
- H01M10/0566—Liquid materials
- H01M10/0568—Liquid materials characterised by the solutes
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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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Abstract
本发明公开一种宽温区不燃的锂离子电池电解液,属于锂离子电池研究领域。这种宽温区不燃的锂离子电池电解液,包括锂盐和聚醚及其衍生物有机溶剂。其特征在于:聚醚及其衍生物有机溶剂作为锂离子电池的溶剂,替代传统的碳酸酯类易燃溶剂。部分聚醚及其衍生物具有很低的熔点,温度在-80℃环境中依然为液态,并且高温200℃仍然稳定存在。本发明提供了一种锂离子电池的电解液与传统电解液相比,在较宽的温度范围内(—40~80℃)表现出较高的离子电导率,闪点燃点高。作为常规电池的电解液在宽温下表现优异的比容量,循环性能以及安全性。
Description
技术领域
本发明提供一种宽温区不燃的锂离子电池电解液,是一种锂离子电池不燃的电解液,属于电化学技术领域。
背景技术
目前,锂离子电解液中主要由容易挥发、低闪点的有机溶液作为溶剂,例如,碳酸乙烯酯、碳酸二甲酯、碳酸二乙酯等;还包含由低分解温度的锂盐作为溶质,例如六氟磷酸锂等。这些都是易燃、易爆的化学物质。对锂离子电池的安全性能有很大的影响。严重的妨碍了锂离子电池在汽车动力电池、航空航天、移动基站等大规模的应用。迄今为止,提高锂离子电池安全性能通常的办法是向电解液中加入阻燃添加剂,比如烷基磷酸酯、氟化磷酸酯、卤代环状碳酸酯、卤代链状碳酸酯。这些虽然能够降低电解液的可燃性,但是在大规模锂电池堆中,阻燃效果有限。仍然能够燃烧。
部分聚醚及其衍生物具有不燃性,即使暴露在空气中使用时,超过400℃才开始缓慢分解,对腐蚀性极强的酸、碱、氧化剂等即使在高温条件下仍然很稳定,对其它几乎所有化学品都比较稳定。部分聚醚及其衍生物是一种常温下为液体的合成聚合物.作为太空机械元器件的润滑剂已有几十年的历史,作为锂离子电池电解液未见报道。另外,部分聚醚及其衍生物具有很低的熔点,温度在-80℃环境中依然为液态,因此解决了锂离子电池低温性能和高温性能。
发明内容
本发明提供一种宽温区不燃的锂离子电池电解液,具有工作温度宽、电池高、低温性能良好特点,解决了常规锂离子电池电解液燃烧这一弊病。
本发明公开的一种宽温区不燃的锂离子电池电解液,其特点在于:
电解液包括有了锂盐、聚醚及其衍生物为电解液溶剂;所述的聚醚及其衍生物具有以下结构式:
Rˊ-CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2-R;
其中,
R为羟基、羧基、烷基直链碳酸酯基、环状碳酸酯基、烷基直链羧酸酯基、环状羧酸酯基、含硫酯基的一种;
Rˊ为羟基、羧基、烷基直链碳酸酯基、环状碳酸酯基、烷基直链羧酸酯基、环状羧酸酯基、含硫酯基的一种;
X为H、F、Cl、Br的一种;
Y为H、F、Cl、Br的一种;
m,n数值为:100-5000。
本发明所述的一种宽温区不燃的锂离子电池电解液,其特征在于:
R、Rˊ为-R1-OH、-R1-COOH、-R1-O-CO-O-R2- 、-R1-O-CO-R2-、-R1-O-SO-O-R2-中的至少一种。
本发明所述的一种宽温区不燃的锂离子电池电解液,其特征在于:
R1、R2为甲基、乙基、丙基、异丙基、丁基中的一种;
R和Rˊ可以为同种基团也可以为不同种基团。
本发明所述电解液的锂盐优选为:三氟甲基磺酸锂、二(三氟甲基磺酸)亚胺锂、三(三氟甲基磺酰)甲基锂(LiCF3SO3、LiN(CF3SO2)2、LiC(SO2CF3)3)中的至少一种。
所述电解液的锂盐浓度:三氟甲基磺酸锂的浓度0. 1-5mol/L;二(三氟甲基磺酸)亚胺锂的浓度0.1-5mol/L;三(三氟甲基磺酰)甲基锂的浓度0. 1-5mol/L。在此浓度范围内,上述的锂盐能很好的实现本发明。
本发明公开的一种宽温区不燃的锂离子电池电解液的制备方法,包括以下步骤:在无氧无水条件下,将聚醚与碳酸二甲酯或碳酸甲乙酯按比例溶解,或通过终端基团反应相连达到均匀溶液,再溶入一定摩尔浓度的锂盐包括三氟甲基磺酸锂、二(三氟甲基磺酸)亚胺锂、三(三氟甲基磺酰)甲基锂中的一种。
所述的一种宽温区不燃的锂离子电池电解液,其特征在于:可用于锂一次电池,锂二次电池。
上述常见有机锂盐阴离子半径大,电荷分布比较分散,电子离域化作用强,这样就减小了锂盐的晶格能,削弱了阴阳离子间的缔合作用,增大溶解度、提高电解液电导率也有利于电化学和热稳定的提高。
本发明的电解液的积极效果在于:配方中有机溶剂通过引入不燃聚醚及其衍生物和高稳定性的锂盐作为锂离子电池电解液的溶质和锂盐,解决了锂离子电池易燃易爆问题、达到高低温性能稳定。对于锂离子电池大规模的应用具有重大的作用。在较宽的液态温度范围内,表现较高的锂离子迁移率;与活性物质,集流体,隔膜不反应,表现出极好的化学稳定性;正负极上表现良好的电化学稳定性,分解电压高;闪点,燃点高,安全性能好;无毒性产物,环境友好型。本发明电池电解液无需添加任何辅助添加剂,可应用于一次、二次锂离子电池。
具体实施方式:
为了使本发明的目的和技术方案及优点更加清楚,本发明用以下具体实施例进行说明,但是本发明并不局限于这些例子。
对比试验:组装正极为磷酸亚铁锂负极为石墨的小型软包锂离子电池,常规电解液为LiPF6/ EC:DEC=1:1, 1C倍率放电,常温25 ℃容量为1358mAH,零下20℃容量为883 mAH,高温60℃容量为1426 mAH。
实施例1
在无氧无水条件下,将聚醚Rˊ-CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2-R,其中,R, Rˊ为-OH(羟基),m=n=5000;与碳酸二甲酯按1:2比例溶解,再溶入三氟甲基磺酸锂摩尔浓度为0.1mol/L。该电解液不燃耐温范围-30---90℃,组装扣式电池常温25℃容量为980 mAH,低温零下30℃容量为810 mAH,高温80℃容量为1045 mAH。
实施例2
在无氧无水条件下,将聚醚Rˊ-CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2-R, 其中,R, Rˊ为CH3-O-COO-,即为H3C-O-COO -CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2- O-COOCH3,X=Y=F(氟 ), m=n=1500;再溶入1.5 mol/L二(三氟甲基磺酸)亚胺锂。该电解液不燃耐温范围-80---300℃,组装扣式电池常温25℃容量为1248 mAH,低温零下40℃容量为1020 mAH,高温90℃容量为1281 mAH。
实施例3
在无氧无水条件下,聚醚Rˊ-CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2-R,其中R, Rˊ为CH3-O-COO-,即为H3C-O-COO -CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2- O-COOCH3,X=Y=Cl(氯), m=n=1000;再溶入1.0mol/L二(三氟甲基磺酸)亚胺锂。该电解液不燃耐温范围-70---300℃,组装扣式电池常温25℃容量为1183 mAH,低温零下40℃容量为946 mAH,高温90℃容量为1201 mAH。
实施例4
在无氧无水条件下,将聚醚Rˊ-CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2-R,其中,R, Rˊ为CH3-O-COO-),即为H3C-O-COO -CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2- O-COOCH3,X=Y=Br, m=n=2000;再溶入三氟甲基磺酸锂摩尔浓度为0.8mol/L。该电解液不燃耐温范围-60---300℃,组装扣式电池常温25℃容量为1168 mAH,低温零下40 ℃容量为980 mAH,高温90℃容量为1205 mAH。
实施例5
在无氧无水条件下,将聚醚Rˊ-CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2-R, 其中R-COOH, Rˊ为CH3-O-COO-,即为
H3C-O-COO -CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2- O-COOH,X=F(氟 ),Y=Cl(氯), m=1000,n=1500;再溶入1.2 mol/L三(三氟甲基磺酰)甲基锂。该电解液不燃耐温范围-70---300℃,组装扣式电池常温25℃容量为1038 mAH,低温零下40℃容量为840 mAH,高温80℃容量为1078 mAH。
实施例6
在无氧无水条件下,将聚醚Rˊ-CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2-R,其中,R, Rˊ为-COOCH2CH3,X=Y=F(氟 ),m=n=5000;与碳酸甲乙酯按1:2比例溶解,再溶入摩尔浓度为3mol/L三氟甲基磺酸锂。该电解液耐温范围-50---100℃,组装扣式电池常温25℃容量为1305 mAH,低温零下30℃容量为1044 mAH,高温80℃容量为1336 mAH。
实施例7
在无氧无水条件下,将聚醚Rˊ-CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2-R,其中,R, Rˊ为-CH2-O-SO-O-CH2CH-,X=Y=F(氟 ),m=n=100;与碳酸甲乙酯按1:3比例溶解,再溶入摩尔浓度为5mol/L三氟甲基磺酸锂。该电解液不燃耐温范围-50---100℃,组装扣式电池常温25℃容量为1158 mAH,低温零下30℃容量为984 mAH,高温80℃容量为1211 mAH。
自上述实施例可见,本发明电解液在常温环境中容量与常规电解液相差不多,但是高温性能、低温性能优异,而且,使用该聚醚及其衍生物具有不燃性,常规电解液则迅速燃烧。由此可见,本发明电解液是解决锂离子电池的安全性问题的有效途径,具有良好的市场价值。
Claims (7)
1.一种不燃的锂离子电池电解液,其特征在于:电解液包括有了锂盐、聚醚及其衍生物为电解液溶剂;
其中聚醚及其衍生物具有以下结构式:
Rˊ-CX2-CY2-(CY2CY2O)m-/-(CY2O)n-CY2-CX2-R
其中,
R为羟基、羧基、烷基直链碳酸酯基、环状碳酸酯基、烷基直链羧酸酯基、环状羧酸酯基、含硫酯基的一种;
Rˊ为羟基、羧基、烷基直链碳酸酯基、环状碳酸酯基、烷基直链羧酸酯基、环状羧酸酯基、含硫酯基的一种;
X为H、F、Cl、Br的一种;
Y为H、F、Cl、Br的一种;
m,n数值为:100-5000。
2. 根据权利要求1所述的一种不燃的锂离子电池电解液,其特征在于:
R、Rˊ为-R1-OH、-R1-COOH、-R1-O-CO-O-R2- 、-R1-O-CO-R2-、-R1-O-SO-O-R2-中的至少一种。
3. 根据权利要求2所述的一种不燃的锂离子电池电解液,其特征在于:
R1、R2为甲基、乙基、丙基、异丙基、丁基中的一种。
4. 根据权利要求2或3中所述,其特征在于:
R和Rˊ可以为同种基团也可以为不同种基团。
5. 根据权利要求1所述的一种不燃的锂离子电池电解液,其特征在于:
所述电解液的锂盐为:三氟甲基磺酸锂、二(三氟甲基磺酸)亚胺锂、三(三氟甲基磺酰)甲基锂(LiCF3SO3、LiN(CF3SO2)2、LiC(SO2CF3)3)中的至少一种。
6. 根据权利要求5所述,其特征在于:
所述电解液的锂盐浓度:三氟甲基磺酸锂的浓度0.1-5mol/L;二(三氟甲基磺酸)亚胺锂的浓度0.1-5mol/L;三(三氟甲基磺酰)甲基锂的浓度0. 1-5mol/L。
7. 权利要求1~7所述的一种不燃的锂离子电池电解液,其特征在于:可用于
锂一次电池,锂二次电池。
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