CN112467220A - 一种适用于硅碳体系锂离子电池的电解液 - Google Patents
一种适用于硅碳体系锂离子电池的电解液 Download PDFInfo
- Publication number
- CN112467220A CN112467220A CN202011396207.7A CN202011396207A CN112467220A CN 112467220 A CN112467220 A CN 112467220A CN 202011396207 A CN202011396207 A CN 202011396207A CN 112467220 A CN112467220 A CN 112467220A
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- Prior art keywords
- electrolyte
- ion battery
- lithium
- lithium ion
- carbonate
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 239000003792 electrolyte Substances 0.000 title claims abstract description 47
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 42
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 37
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 title claims abstract description 29
- 239000000654 additive Substances 0.000 claims abstract description 22
- SBLRHMKNNHXPHG-UHFFFAOYSA-N 4-fluoro-1,3-dioxolan-2-one Chemical compound FC1COC(=O)O1 SBLRHMKNNHXPHG-UHFFFAOYSA-N 0.000 claims abstract description 14
- 230000000996 additive effect Effects 0.000 claims abstract description 14
- 229910003002 lithium salt Inorganic materials 0.000 claims abstract description 10
- 159000000002 lithium salts Chemical class 0.000 claims abstract description 10
- 125000002023 trifluoromethyl group Chemical group FC(F)(F)* 0.000 claims abstract description 10
- 239000003960 organic solvent Substances 0.000 claims abstract description 9
- RIUWBIIVUYSTCN-UHFFFAOYSA-N trilithium borate Chemical compound [Li+].[Li+].[Li+].[O-]B([O-])[O-] RIUWBIIVUYSTCN-UHFFFAOYSA-N 0.000 claims abstract description 7
- -1 lithium trifluoromethyltriethylborate Chemical compound 0.000 claims description 17
- FKRCODPIKNYEAC-UHFFFAOYSA-N ethyl propionate Chemical compound CCOC(=O)CC FKRCODPIKNYEAC-UHFFFAOYSA-N 0.000 claims description 8
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 claims description 6
- UHOPWFKONJYLCF-UHFFFAOYSA-N 2-(2-sulfanylethyl)isoindole-1,3-dione Chemical compound C1=CC=C2C(=O)N(CCS)C(=O)C2=C1 UHOPWFKONJYLCF-UHFFFAOYSA-N 0.000 claims description 4
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 4
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 claims description 4
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 4
- 229920001774 Perfluoroether Polymers 0.000 claims description 4
- 150000001733 carboxylic acid esters Chemical class 0.000 claims description 4
- 229910052744 lithium Inorganic materials 0.000 claims description 4
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 4
- VTHRQKSLPFJQHN-UHFFFAOYSA-N 3-[2-(2-cyanoethoxy)ethoxy]propanenitrile Chemical compound N#CCCOCCOCCC#N VTHRQKSLPFJQHN-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
- WVCXIIOIWJECBJ-UHFFFAOYSA-N FC(CF)(F)C(C(C(F)(F)F)(F)F)OC(C(C(F)(F)F)(F)F)C(CF)(F)F Chemical group FC(CF)(F)C(C(C(F)(F)F)(F)F)OC(C(C(F)(F)F)(F)F)C(CF)(F)F WVCXIIOIWJECBJ-UHFFFAOYSA-N 0.000 claims description 2
- BTGRAWJCKBQKAO-UHFFFAOYSA-N adiponitrile Chemical compound N#CCCCCC#N BTGRAWJCKBQKAO-UHFFFAOYSA-N 0.000 claims description 2
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 claims description 2
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 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 description 2
- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 claims description 2
- IAHFWCOBPZCAEA-UHFFFAOYSA-N succinonitrile Chemical compound N#CCCC#N IAHFWCOBPZCAEA-UHFFFAOYSA-N 0.000 claims description 2
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- KLLQVNFCMHPYGL-UHFFFAOYSA-N 5h-oxathiole 2,2-dioxide Chemical group O=S1(=O)OCC=C1 KLLQVNFCMHPYGL-UHFFFAOYSA-N 0.000 description 2
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- 101150058243 Lipf gene Proteins 0.000 description 2
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 2
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- GVGUFUZHNYFZLC-UHFFFAOYSA-N dodecyl benzenesulfonate;sodium Chemical compound [Na].CCCCCCCCCCCCOS(=O)(=O)C1=CC=CC=C1 GVGUFUZHNYFZLC-UHFFFAOYSA-N 0.000 description 2
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- XQSBLCWFZRTIEO-UHFFFAOYSA-N hexadecan-1-amine;hydrobromide Chemical compound [Br-].CCCCCCCCCCCCCCCC[NH3+] XQSBLCWFZRTIEO-UHFFFAOYSA-N 0.000 description 2
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- 239000002000 Electrolyte additive Substances 0.000 description 1
- 229910032387 LiCoO2 Inorganic materials 0.000 description 1
- 229910052493 LiFePO4 Inorganic materials 0.000 description 1
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- 229910002097 Lithium manganese(III,IV) oxide Inorganic materials 0.000 description 1
- 229910014514 LixNiyM1-yO2 Inorganic materials 0.000 description 1
- 229910014512 LixNiyM1−yO2 Inorganic materials 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 239000006183 anode active material Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052791 calcium Inorganic materials 0.000 description 1
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- LNLFLMCWDHZINJ-UHFFFAOYSA-N hexane-1,3,6-tricarbonitrile Chemical compound N#CCCCC(C#N)CCC#N LNLFLMCWDHZINJ-UHFFFAOYSA-N 0.000 description 1
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- VDVLPSWVDYJFRW-UHFFFAOYSA-N lithium;bis(fluorosulfonyl)azanide Chemical compound [Li+].FS(=O)(=O)[N-]S(F)(=O)=O VDVLPSWVDYJFRW-UHFFFAOYSA-N 0.000 description 1
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Classifications
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- H01M10/05—Accumulators with non-aqueous electrolyte
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- H—ELECTRICITY
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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
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- 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
- Y02E60/10—Energy storage using batteries
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Inorganic Chemistry (AREA)
- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
- Physics & Mathematics (AREA)
- Composite Materials (AREA)
- Materials Engineering (AREA)
- Secondary Cells (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
本发明提供一种适用于硅碳体系锂离子电池的电解液及包括该电解液的硅碳体系锂离子电池。本发明中提供的电解液包括有机溶剂、添加剂和锂盐,所述添加剂包括三氟甲基三乙基硼酸锂、丙烯基‑1,3‑磺酸内酯和氟代碳酸乙烯酯,该添加剂组合使用可以显著提升硅碳电池的循环寿命,同时兼顾高低温性能和安全性能,从而使硅碳电池更适合大规模商业化生产。
Description
技术领域
本发明属于锂离子电池技术领域,具体涉及一种适用于硅碳体系锂离子电池的电解液。
背景技术
锂离子电池自从商业化以来,由于它的比能量高、循环性能好,被广泛用于数码、储能、动力、军用航天和通讯设备等领域。随着锂离子电池的广泛应用,消费者对锂离子电池的使用环境、需求不断提升,同时对电子设备的续航能力要求越来越高,这就要求锂离子电池具有高低温性能兼顾的同时能够具有较高的能量密度。
硅碳电池是提高电池能量密度的有效手段之一,而其中电解液是硅碳锂离子电池的主材之一,它在硅碳锂离子电池中起到传输Li+的作用。因此,电解液的研究与开发对硅碳锂离子电池来说至关重要,然而缓解硅负极循环膨胀大和兼顾高低温性能的电解液并不容易开发。现阶段,电解液中添加剂的使用是解决以上问题的高效武器。但是,当前的电解液添加剂往往难以形成坚固有韧性的SEI膜来抵挡循环过程中硅负极膨胀带来的破坏,且高温添加剂带来的阻抗较大,且严重影响了电池的低温性能。因此,迫切需要开发一种能够延长硅碳电池循环寿命以及高低温兼顾的适用于硅碳体系锂离子电池的电解液。
发明内容
本发明提供了一种适用于硅碳体系锂离子电池的电解液,使用该电解液的硅碳锂离子电池可以有效缓解电池循环膨胀大、电池循环寿命低和电池高低温性能难兼顾等问题,从而显著提升硅碳体系锂离子电池的高低温性能和循环寿命,此外还能显著提升硅碳体系锂离子电池的安全性能,适合大规模商业化生产。
具体的,本发明提供了如下技术方案:
一种适用于硅碳体系锂离子电池的电解液,其中,所述电解液包括有机溶剂、添加剂和锂盐,所述添加剂包括三氟甲基三乙基硼酸锂、丙烯基-1,3-磺酸内酯和氟代碳酸乙烯酯。
进一步地,所述三氟甲基三乙基硼酸锂的使用量占电解液总质量的0.1-2wt%,优选为0.2-1.0wt%,再优选为0.2-0.5wt%,例如为0.1wt%、0.2wt%、0.3wt%、0.4wt%、0.5wt%、0.8wt%、0.9wt%、1wt%、1.2wt%、1.3wt%、1.4wt%、1.5wt%、1.6wt%、1.7wt%、1.8wt%、1.9wt%或2.0wt%。
本发明中,所述的三氟甲基三乙基硼酸锂可以通过本领域已知的方法制备得到,也可以通过商业途径购买获得。
本发明中,所述的三氟甲基三乙基硼酸锂的结构如式1所示:
进一步地,所述丙烯基-1,3-磺酸内酯的使用量占电解液总质量的0.2-3.5wt%,优选为0.5-2wt%,例如为0.2wt%、0.3wt%、0.4wt%、0.5wt%、0.8wt%、0.9wt%、1wt%、1.2wt%、1.3wt%、1.4wt%、1.5wt%、1.6wt%、1.7wt%、1.8wt%、1.9wt%、2.0wt%、3.0wt%或3.5wt%。
本发明中,所述的丙烯基-1,3-磺酸内酯的英文名称为prop-1-ene-1,3-sultone,其CAS号:21806-61-1,其可以通过本领域已知的方法制备得到,也可以通过商业途径购买获得。
进一步地,所述氟代碳酸乙烯酯的使用量占电解液总质量的8-20wt%,例如为8wt%、9wt%、10wt%、11wt%、12wt%、13wt%、14wt%、15wt%、16wt%、17wt%、18wt%、19wt%或20wt%。
本发明中,所述的氟代碳酸乙烯酯的英文名称为fluoroethylene carbonate,其CAS号:114435-02-8,其可以通过本领域已知的方法制备得到,也可以通过商业途径购买获得。
进一步地,所述添加剂还包括丁二腈、己二腈、甘油三腈、1,3,6-己烷三腈和1,2-双(氰乙氧基)乙烷中的至少一种,其使用量占电解液总质量的0-10wt%;示例性的可以为1-5wt%。
进一步地,所述有机溶剂选自碳酸酯、羧酸酯和氟代醚中的至少一种,其中,所述的碳酸酯选自碳酸乙烯酯、碳酸丙烯酯、碳酸二甲酯、碳酸甲乙酯、碳酸二乙酯、碳酸甲丙酯中的一种或多种组合;所述的羧酸酯选自丙酸乙酯、丙酸丙酯中的一种或多种组合;所述的氟代醚选自1,1,2,3-四氟乙基-2,2,3,3-四氟丙基醚。
进一步地,所述锂盐选自六氟磷酸锂、双氟磺酰亚胺锂或双(三氟甲基磺酰)亚胺锂中的一种或多种。
进一步地,所述锂盐的使用量占电解液总质量的10-20wt%,例如为10wt%、11wt%、12wt%、13wt%、14wt%、15wt%、16wt%、17wt%、18wt%、19wt%或20wt%。
本发明还提供一种电解液的制备方法,所述方法包括如下步骤:
将有机溶剂、添加剂和锂盐混合,其中,所述添加剂包括三氟甲基三乙基硼酸锂、丙烯基-1,3-磺酸内酯和氟代碳酸乙烯酯。
示例性地,所述方法包括如下步骤:
在充满氩气水氧含量合格的手套箱中,准备有机溶剂,然后往其中快速加入充分干燥的锂盐、三氟甲基三乙基硼酸锂、丙烯基-1,3-磺酸内酯和氟代碳酸乙烯酯,制备得到所述电解液。
本发明还提供一种锂离子电池,所述锂离子电池包括上述的电解液。
进一步地,所述锂离子电池为硅碳体系锂离子电池。
进一步地,所述锂离子电池还包括正极片、负极片和隔膜。
进一步地,所述负极片包括负极集流体和涂覆在负极集流体一侧或两侧表面的负极活性物质层,其中,所述负极活性物质层中包括负极活性物质,所述负极活性物质选自纳米硅和/或SiOx(0.8≤x≤1.3)与石墨复合而成的硅碳负极材料。
进一步地,所述纳米硅和/或SiOx占硅碳负极材料总质量的1-55wt%,如1wt%、2wt%、5wt%、8wt%、10wt%、12wt%、15wt%、18wt%、20wt%、25wt%、30wt%、35wt%、40wt%、45wt%、50wt%、55wt%。
进一步地,所述负极活性物质层还包括粘结剂、导电剂和分散剂。
进一步地,所述负极活性物质层中各组分的质量百分含量为:负极活性物质70-99.7wt%,粘结剂0.1-10wt%、分散剂0.1-10wt%、导电剂0.1-10wt%。
优选地,所述负极活性物质层中各组分的质量百分含量为:负极活性物质76-98.5wt%,粘结剂0.5-8wt%、分散剂0.5-8wt%、导电剂0.5-8wt%。
还优选地,所述负极活性物质层中各组分的质量百分含量为:负极活性物质85-98.5wt%,粘结剂0.5-5wt%、分散剂0.5-5wt%、导电剂0.5-5wt%。
进一步地,所述粘结剂选自聚偏氟乙烯(PVDF)、聚四氟乙烯(PTFE)、聚乙烯亚胺(PEI)、聚苯胺(PAN)、聚丙烯酸(PAA)、海藻酸钠、丁苯橡胶(SBR)、羧甲基纤维素钠(CMC)、酚醛树脂或环氧树脂等高分子聚合物中的至少一种。
进一步地,所述分散剂选自聚丙烯(PVA)、十六烷基溴化铵、十二烷基苯磺酸钠、硅烷偶联剂、乙醇、N-甲基吡咯烷酮(NMP)、N,N-二甲基甲酰胺(DMF)等的至少一种,更优选地为十六烷基溴化铵、十二烷基苯磺酸钠、硅烷偶联剂、乙醇中的至少一种。
进一步地,所述导电剂选自碳纳米管(CNTs)、碳纤维(VGCF)、导电石墨(KS-6、SFG-6)、中间相碳微球(MCMB)、石墨烯、科琴黑、Super P、乙炔黑、导电炭黑或硬碳中的至少一种。
进一步地,所述正极片包括正极集流体和涂覆在正极集流体一侧或两侧表面的正极活性物质层,其中,所述正极活性物质层中包括正极活性物质,所述正极活性物质选自LiCoO2、LiNiO2、LiMn2O4、LiFePO4、LixNiyM1-yO2中的一种或几种,其中,0.9≤x≤1.2,0.5≤y<1,M选自Co、Mn、Al、Mg、Ti、Zr、Fe、Cr、Mo、Cu、Ca中的一种或几种。
进一步地,所述正极活性物质层还包括粘结剂和导电剂。
进一步地,所述正极活性物质层中各组分的质量百分含量为:正极活性物质80-99.8wt%,粘结剂0.1-10wt%、导电剂0.1-10wt%。
优选地,所述正极活性物质层中各组分的质量百分含量为:正极活性物质84-99wt%,粘结剂0.5-8wt%、导电剂0.5-8wt%。
还优选地,所述正极活性物质层中各组分的质量百分含量为:正极活性物质90-99wt%,粘结剂0.5-5wt%、导电剂0.5-5wt%。
进一步地,所述粘结剂选自聚偏氟乙烯(PVDF)、聚四氟乙烯(PTFE)、聚乙烯亚胺(PEI)、聚苯胺(PAN)、聚丙烯酸(PAA)、海藻酸钠、丁苯橡胶(SBR)、羧甲基纤维素钠(CMC)、酚醛树脂或环氧树脂等高分子聚合物中的至少一种。
进一步地,所述导电剂选自碳纳米管(CNTs)、碳纤维(VGCF)、导电石墨(KS-6、SFG-6)、中间相碳微球(MCMB)、石墨烯、科琴黑、Super P、乙炔黑、导电炭黑或硬碳中的至少一种。
进一步地,所述隔膜为本领域已知的隔膜,例如为聚乙烯隔膜、聚丙烯隔膜等。
本发明还提供上述锂离子电池的制备方法,所述方法包括如下步骤:
(1)准备正极片和负极片,所述正极片中含有正极活性物质,所述负极片中含有负极活性物质;
(2)将有机溶剂、添加剂和锂盐混合,制备得到电解液;
(3)将正极片、隔膜、负极片通过卷绕得到未注液的裸电芯;将裸电芯置于外包装箔中,将步骤(2)的电解液注入到干燥后的裸电芯中,制备得到所述锂离子电池。
示例性地,所述方法具体包括如下步骤:
(1)正极片制备
将正极活性物质LiCoO2、粘结剂聚偏氟乙烯(PVDF)、导电剂乙炔黑按照重量比96.5:2:1.5进行混合,加入N-甲基吡咯烷酮(NMP),在真空搅拌机作用下搅拌,直至混合体系成均一流动性的正极浆料;将正极浆料均匀涂覆于厚度为9~12μm的铝箔上;将上述涂覆好的铝箔在5段不同温度梯度的烘箱烘烤后,再将其在120℃的烘箱干燥8h,然后经过辊压、分切得到所需的正极片。
(2)硅碳负极片制备
将质量占比为95.9%的硅碳负极材料(采用SiO与石墨复合而成,SiO质量占比3%),质量占比为0.1%的单壁碳纳米管(SWCNT)导电剂、质量占比为1%的导电炭黑(SP)导电剂、质量占比为1%的羧甲基纤维素钠(CMC)分散剂及质量占比为2%的丁苯橡胶(SBR)粘结剂以湿法工艺制成负极浆料;将负极浆料均匀涂覆于厚度为9~12μm的铜箔上;将上述涂覆好的铜箔在5段不同温度梯度的烘箱烘烤后,再将其在85℃的烘箱干燥5h,然后经过辊压、分切得到所需的硅碳负极片。
(3)电解液制备
在充满氩气水氧含量合格的手套箱中,将碳酸乙烯酯、碳酸丙烯酯、丙酸丙酯和丙酸乙酯按照质量比1:2:5:2的比例混合均匀(溶剂需要归一化),然后往其中快速加入1mol/L(12.5wt%)的充分干燥的六氟磷酸锂(LiPF6)、添加剂(包括三氟甲基三乙基硼酸锂、丙烯基-1,3-磺酸内酯和氟代碳酸乙烯酯等),得到电解液。
(4)隔膜的制备
选用7~9μm厚的聚乙烯隔膜。
(5)锂离子电池的制备
将上述准备的正极片、隔膜、负极片通过卷绕得到未注液的裸电芯;将裸电芯置于外包装箔中,将上述制备好的电解液注入到干燥后的裸电芯中,经过真空封装、静置、化成、整形、分选等工序,获得所需的锂离子电池。
本发明的有益效果:
本发明提供的电解液中氟代碳酸乙烯酯和三氟甲基三乙基硼酸锂联用可以在硅碳负极表面形成坚韧的低阻抗SEI复合膜,对硅碳负极材料的循环膨胀有明显抑制作用,可以延长电池的循环寿命,同时还使得锂离子能够更易可逆脱出/嵌入,从而提高了电池的低温性能。丙烯基-1,3-磺酸内酯与三氟甲基三乙基硼酸锂联用能够在正负极表面生成更坚固的复合保护膜,有效提升电池的高温性能和安全性。本发明将三种添加剂组合使用,通过三者的协同作用可以显著提升硅碳电池的循环寿命,同时兼顾高低温性能和安全性能。
具体实施方式
下文将结合具体实施例对本发明做更进一步的详细说明。应当理解,下列实施例仅为示例性地说明和解释本发明,而不应被解释为对本发明保护范围的限制。凡基于本发明上述内容所实现的技术均涵盖在本发明旨在保护的范围内。
下述实施例中所使用的实验方法如无特殊说明,均为常规方法;下述实施例中所用的试剂、材料等,如无特殊说明,均可从商业途径得到。
对比例1-6和实施例1-8
对比例1-6和实施例1-8的锂离子电池均按照下述制备方法进行制备,区别仅在于电解液中的各组分的选择和加入量不同,具体区别如表1所示。
(1)正极片制备
将正极活性物质LiCoO2、粘结剂聚偏氟乙烯(PVDF)、导电剂乙炔黑按照重量比96.5:2:1.5进行混合,加入N-甲基吡咯烷酮(NMP),在真空搅拌机作用下搅拌,直至混合体系成均一流动性的正极浆料;将正极浆料均匀涂覆于厚度为9~12μm的铝箔上;将上述涂覆好的铝箔在5段不同温度梯度的烘箱烘烤后,再将其在120℃的烘箱干燥8h,然后经过辊压、分切得到所需的正极片。
(2)硅碳负极片制备
将质量占比为95.9%的硅碳负极材料(采用SiO与石墨复合而成,SiO质量占比3%),质量占比为0.1%的单壁碳纳米管(SWCNT)导电剂、质量占比为1%的导电炭黑(SP)导电剂、质量占比为1%的羧甲基纤维素钠(CMC)分散剂及质量占比为2%的丁苯橡胶(SBR)粘结剂以湿法工艺制成负极浆料;将负极浆料均匀涂覆于厚度为9~12μm的铜箔上;将上述涂覆好的铜箔在5段不同温度梯度的烘箱烘烤后,再将其在85℃的烘箱干燥5h,然后经过辊压、分切得到所需的硅碳负极片。
(3)电解液制备
在充满氩气水氧含量合格的手套箱中,将碳酸乙烯酯、碳酸丙烯酯、丙酸丙酯和丙酸乙酯按照质量比1:2:5:2的比例混合均匀(溶剂需要归一化),然后往其中快速加入1mol/L(12.5wt%)的充分干燥的六氟磷酸锂(LiPF6)、质量占比为3wt%的1,3,6-己烷三腈和其他添加剂(包括三氟甲基三乙基硼酸锂、丙烯基-1,3-磺酸内酯和氟代碳酸乙烯酯,具体用量和选择如表1所示),得到电解液。
(4)隔膜的制备
选用7~9μm厚的聚乙烯隔膜。
(5)锂离子电池的制备
将上述准备的正极片、隔膜、负极片通过卷绕得到未注液的裸电芯;将裸电芯置于外包装箔中,将上述制备好的电解液注入到干燥后的裸电芯中,经过真空封装、静置、化成、整形、分选等工序,获得所需的锂离子电池。
表1对比例1-6和实施例1-8的步骤(3)的电解液中的其他添加剂的组成和加入量
对上述对比例和实施例所得电池进行电化学性能测试,相关说明如下:
(1)45℃循环实验:
将上述实施例和对比例所得电池置于(45±2)℃环境中,静置2-3个小时,待电池本体达到(45±2)℃时,电池按照1C恒流充电截止电流为0.05C,电池充满电后搁置5min,再以0.7C恒流放电至截止电压3.0V,记录前3次循环的最高放电容量为初始容量Q,记录电芯初始厚度T,当循环达到所需的次数时,记录电池的最后一次的放电容量Q1和电池厚度T1,记录结果如表2。
其中用到的计算公式如下:
容量保持率(%)=Q1/Q×100%;
厚度变化率(%)=(T1-T)/T×100%。
(2)85℃高温存储10小时实验:
将上述实施例和对比例所得电池置于室温下以0.5C的充放电倍率进行3次充放电循环测试,然后0.5C倍率充到满电状态,分别记录前3次0.5C循环的最高放电容量Q2和电池厚度T2。将满电状态的电池在85℃下存储10小时,记录10小时后的电池厚度T3和0.5C放电容量Q3,计算得到电池高温存储的厚度变化率和容量保持率等实验数据,记录结果如表2。
其中用到的计算公式如下:
容量保持率(%)=Q3/Q2×100%;
厚度变化率(%)=(T3-T2)/T2×100%。
(3)130℃热冲击实验:
将上述实施例和对比例所得电池用对流方式或循环热空气箱以起始温度25±3℃进行加热,温变率5±2℃/min,升温至130±2℃℃,保持60min后结束试验,记录电池状态结果如表2。
(4)低温放电实验:
将上述实施例和对比例所得电池在环境温度25±3℃,先以0.2C放电至3.0V,搁置5min;以0.7C充电,当电芯端电压达到充电限制电压时,改为恒压充电,直到充电电流≤截止电流,停止充电,搁置5分钟后,以0.2C放电至3.0V,记录此次放电容量为常温容量Q4。然后电芯以0.7C充电,当电芯端电压达到充电限制电压时,改为恒压充电,直到充电电流小于或等于截止电流,停止充电;将充满电的电池在-10±2℃条件下搁置4h后,以0.4C电流放电至截止电压3.0V,记录放电容量Q5,计算可得低温放电容量保持率,记录结果如表2。
其中用到的计算公式如下:
低温放电容量保持率(%)=Q5/Q4×100%。
表2对比例1-6和实施例1-8的性能测试结果
由表2结果可以看出:
综上所述,本发明提供的适用于硅碳体系锂离子电池的电解液含有三氟甲基三乙基硼酸锂、丙烯基-1,3-磺酸内酯和氟代碳酸乙烯酯的添加剂组合,通过添加剂之间的协同作用能够使硅碳体系锂离子电池具有优异的高温循环、高温储存和低温放电性能的同时还兼顾高安全性。
以上,对本发明的实施方式进行了说明。但是,本发明不限定于上述实施方式。凡在本发明的精神和原则之内,所做的任何修改、等同替换、改进等,均应包含在本发明的保护范围之内。
Claims (9)
1.一种适用于硅碳体系锂离子电池的电解液,其中,所述电解液包括有机溶剂、添加剂和锂盐,所述添加剂包括三氟甲基三乙基硼酸锂、丙烯基-1,3-磺酸内酯和氟代碳酸乙烯酯。
2.根据权利要求1所述的电解液,其中,所述三氟甲基三乙基硼酸锂的使用量占电解液总质量的0.1-2wt%,优选为0.2-1.0wt%,再优选为0.2-0.5wt%。
3.根据权利要求1或2所述的电解液,其中,所述丙烯基-1,3-磺酸内酯的使用量占电解液总质量的0.2-3.5wt%,优选为0.5-2wt%。
4.根据权利要求1-3任一项所述的电解液,其中,所述氟代碳酸乙烯酯的使用量占电解液总质量的8-20wt%。
5.根据权利要求1-4任一项所述的锂离子电池,其中,所述添加剂还包括丁二腈、己二腈、甘油三腈、1,3,6-己烷三腈和1,2-双(氰乙氧基)乙烷中的至少一种,其使用量占电解液总质量的0-10wt%。
6.根据权利要求1-5任一项所述的锂离子电池,其中,所述有机溶剂选自碳酸酯、羧酸酯和氟代醚中的至少一种,其中,所述的碳酸酯选自碳酸乙烯酯、碳酸丙烯酯、碳酸二甲酯、碳酸甲乙酯、碳酸二乙酯、碳酸甲丙酯中的一种或多种组合;所述的羧酸酯选自丙酸乙酯、丙酸丙酯中的一种或多种组合;所述的氟代醚选自1,1,2,3-四氟乙基-2,2,3,3-四氟丙基醚。
7.根据权利要求1-6任一项所述的锂离子电池,其中,所述锂盐选自六氟磷酸锂、双氟磺酰亚胺锂或双(三氟甲基磺酰)亚胺锂中的一种或多种;和/或,
所述锂盐的使用量占电解液总质量的10-20wt%。
8.一种锂离子电池,其中,所述锂离子电池包括权利要求1-7任一项所述的电解液。
9.根据权利要求8所述的锂离子电池,其中,所述锂离子电池为硅碳体系锂离子电池。
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WO2022227450A1 (zh) * | 2021-04-30 | 2022-11-03 | 宁德新能源科技有限公司 | 电解液、电化学装置和电子装置 |
CN115548444A (zh) * | 2022-11-29 | 2022-12-30 | 瑞浦兰钧能源股份有限公司 | 一种配硅用电解液及含其的电池 |
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