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Article(id=1214642641082437762, tenantId=1146029695717560320, journalId=1189645257101713411, issueId=1214642640251961379, articleNumber=null, orderNo=null, doi=10.19822/j.cnki.1671-6329.20220177, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=null, receivedDateStr=null, revisedDate=null, revisedDateStr=null, acceptedDate=null, acceptedDateStr=null, onlineDate=1767522972602, onlineDateStr=2026-01-04, pubDate=1691164800000, pubDateStr=2023-08-05, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1767522972602, onlineIssueDateStr=2026-01-04, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1767522972602, creator=13701087609, updateTime=1767522972602, updator=13701087609, issue=Issue{id=1214642640251961379, tenantId=1146029695717560320, journalId=1189645257101713411, year='2023', volume='', issue='8', pageStart='1', pageEnd='62', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1767522972404, creator=13701087609, updateTime=1767533854059, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1214688281275585312, tenantId=1146029695717560320, journalId=1189645257101713411, issueId=1214642640251961379, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1214688281275585313, tenantId=1146029695717560320, journalId=1189645257101713411, issueId=1214642640251961379, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=7, endPage=13, ext={EN=ArticleExt(id=1214642641262792836, articleId=1214642641082437762, tenantId=1146029695717560320, journalId=1189645257101713411, language=EN, title=Advances of Binders for Silicon-Based Anodes in Lithium-ion Batteries, columnId=null, journalTitle=Automotive Digest, columnName=null, runingTitle=null, highlight=null, articleAbstract=

Lithium-ion batteries with silicon-based anodes are considered to be the most promising next-generation Lithium-ion batteries due to their high theoretical specific capacity and low operating voltage. However, the inherent huge volume expansion of silicon-based materials after lithiation and the resulting problems seriously restrict the practical application of silicon-based anodes. From different functional types of polymer binders, the latest research progress of binders for silicon-based anodes is summarized. Finally, a method for rationally designing binders for silicon-based anodes and suggestions for industrial production are proposed.

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具有硅基负极的锂离子电池，由于其理论比容量高、工作电压低的优点，被认为是最具前景的下一代锂离子电池。然而，锂化后硅基材料固有的较大体积膨胀以及由此产生的问题，严重制约着硅基负极材料的实际应用。总结了高弹性聚合物黏结剂、自修复聚合物黏结剂和导电聚合物黏结剂3种不同功能类型的聚合物黏结剂，对硅基负极用黏结剂的最新研究现状进行了分析和概述。并在此基础上，提出合理设计硅基负极用黏结剂方法和实现工业化生产建议。

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张玉坤，1988，男，硕士，就职于广汽丰田汽车有限公司，研究方向为新能源汽车电池加工工艺与质量管理。E-mail:

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张玉坤，1988，男，硕士，就职于广汽丰田汽车有限公司，研究方向为新能源汽车电池加工工艺与质量管理。E-mail:

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张玉坤，1988，男，硕士，就职于广汽丰田汽车有限公司，研究方向为新能源汽车电池加工工艺与质量管理。E-mail:

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黏结剂 负极材料 首次放电比容量/ mA·h·g-1 剩余比容量（电池循环次数）/mA·h·g-1 w（AM）/%∶w（ECA）/%∶w（B）/% 参考文献
PVDF Si/C 1 255.9 569.2(50th) 80∶10∶10 [31]
PAA/PDA 纳米Si 3 192.0 1 961.0(100th) 60∶20∶20 [26]
CS-g-PAAA 纳米Si 2 785.6 1 301.0(300th) 60∶20∶20 [48]
CMC/SBR Si 2 250.0 1 750.0(10th) 70∶15∶15 [49]
OS-CMC Si 3 424.0 1 922.0 60∶20∶20 [50]
SHP-PEG Si 1 400.0 1 300.0(150th) 65∶30∶5 [38]
PFM SiOx/C 1 500.0 750.0(40th) 80∶5∶15 [43]
PSSA@PANI 纳米Si 4 353.5 1 790.2(100th) 70∶15∶15 [44]
三元黏结剂 纳米Si 2 026.0 1 620.8 60∶10∶20 [45]
), ArticleFig(id=1215266500106179405, tenantId=1146029695717560320, journalId=1189645257101713411, articleId=1214642641082437762, language=CN, label=表1, caption=

不同黏结剂电池性能对比

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黏结剂 负极材料 首次放电比容量/ mA·h·g-1 剩余比容量（电池循环次数）/mA·h·g-1 w（AM）/%∶w（ECA）/%∶w（B）/% 参考文献
PVDF Si/C 1 255.9 569.2(50th) 80∶10∶10 [31]
PAA/PDA 纳米Si 3 192.0 1 961.0(100th) 60∶20∶20 [26]
CS-g-PAAA 纳米Si 2 785.6 1 301.0(300th) 60∶20∶20 [48]
CMC/SBR Si 2 250.0 1 750.0(10th) 70∶15∶15 [49]
OS-CMC Si 3 424.0 1 922.0 60∶20∶20 [50]
SHP-PEG Si 1 400.0 1 300.0(150th) 65∶30∶5 [38]
PFM SiOx/C 1 500.0 750.0(40th) 80∶5∶15 [43]
PSSA@PANI 纳米Si 4 353.5 1 790.2(100th) 70∶15∶15 [44]
三元黏结剂 纳米Si 2 026.0 1 620.8 60∶10∶20 [45]
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锂离子电池硅基负极用黏结剂研究进展
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张玉坤 , 邹朝辉 , 张云霞
汽车文摘 | 2023,(8): 7-13
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汽车文摘 | 2023, (8): 7-13
锂离子电池硅基负极用黏结剂研究进展
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张玉坤 , 邹朝辉, 张云霞
作者信息
  • 广汽丰田汽车有限公司， 广州 511455

    • 张玉坤，1988，男，硕士，就职于广汽丰田汽车有限公司，研究方向为新能源汽车电池加工工艺与质量管理。E-mail:

Advances of Binders for Silicon-Based Anodes in Lithium-ion Batteries
Yukun Zhang , Zhaohui Zou, Yunxia Zhang
Affiliations
  • GAC Toyota Motor Co., Ltd, Guangzhou 511455
出版时间: 2023-08-05 doi: 10.19822/j.cnki.1671-6329.20220177
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摘要
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具有硅基负极的锂离子电池，由于其理论比容量高、工作电压低的优点，被认为是最具前景的下一代锂离子电池。然而，锂化后硅基材料固有的较大体积膨胀以及由此产生的问题，严重制约着硅基负极材料的实际应用。总结了高弹性聚合物黏结剂、自修复聚合物黏结剂和导电聚合物黏结剂3种不同功能类型的聚合物黏结剂，对硅基负极用黏结剂的最新研究现状进行了分析和概述。并在此基础上，提出合理设计硅基负极用黏结剂方法和实现工业化生产建议。

锂离子电池  /  硅基负极  /  黏结剂  /  聚合物  /  新能源汽车

Lithium-ion batteries with silicon-based anodes are considered to be the most promising next-generation Lithium-ion batteries due to their high theoretical specific capacity and low operating voltage. However, the inherent huge volume expansion of silicon-based materials after lithiation and the resulting problems seriously restrict the practical application of silicon-based anodes. From different functional types of polymer binders, the latest research progress of binders for silicon-based anodes is summarized. Finally, a method for rationally designing binders for silicon-based anodes and suggestions for industrial production are proposed.

Lithium ion battery  /  Silicon-based anode  /  Binder  /  Polymer  /  New energy vehicle
张玉坤, 邹朝辉, 张云霞. 锂离子电池硅基负极用黏结剂研究进展. 汽车文摘, 2023 , (8) : 7 -13 . DOI: 10.19822/j.cnki.1671-6329.20220177
Yukun Zhang, Zhaohui Zou, Yunxia Zhang. Advances of Binders for Silicon-Based Anodes in Lithium-ion Batteries[J]. Automotive Digest, 2023 , (8) : 7 -13 . DOI: 10.19822/j.cnki.1671-6329.20220177
正文
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缩略语
PVDF Polyvinylidene Fluoride
PAA Polyacrylic Acid
SBR Styrene Butadiene Rubber
CMC Carboxymethyl Cellulose
PDA Polydopamine
4A-PAA Four-Armed Polyacrylic Acid
CS Chitosan
SHP Self-Healing Polymer
UPy Ureidopyrimidinone
PEG Polyethylene Glycol
APS Ammonium Persulfate
AN Aniline
PSSA Polystyrene Sulfonic Acid
PVA Polyvinyl Alcohol
PAAA Poly(aniline-co-anthranilic acid)
OS-CMC Oxidized Starch Cross-linked
Sodium Carboxymethyl Cellulose
PETU Poly(Ether-Thioureas)
PFM Poly(9,9-dioctylfluorene-co-fluore
nonecomethylbenzoic ester)
PEDOT:PSS Poly(3,4-ethylenedioxythiophene):
Poly(styrene sulfonate)
0 引言
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近年来，新能源汽车因运行时能量损失少、环境污染少的优点，市场持续爆发式增长[1-2]，2022年市场渗透率达25.6%。其中，锂离子电池因其具有更高的能量密度、更长的循环寿命和更高的电压优势，在新能源汽车领域应用最为广泛[3-5]。但是，随着新能源汽车市场的迅速发展，对锂离子电池也提出了更大可逆容量、更大倍率容量和更长循环寿命的需求[6]。
为了满足锂离子电池不断增长的需求，由于硅具有高比容量、低工作电压以及资源丰富和环境友好的优点，被用于开发下一代负极材料[7-8]。但是，硅基电极的大规模推广应用尚存在一些困难，其中最大的阻碍是其在循环过程中300%的体积膨胀，会导致颗粒破碎并破坏电极结构，从而导致容量快速衰减[9-11]。在过去的研究中，有很多方法用于限制循环期间硅基电极的体积膨胀，如减少硅的粒径，硅表面涂层和制造硅基复合材料等[12-15]。此外，还发现聚合物黏合剂可以有效提高硅基电极的循环寿命和能量密度，这是由于聚合物黏结剂，通过与硅表面的-OH基团的强化学相互作用（氢键和共价键），有助于在循环过程中保持硅基电极的完整性[16-18]。
聚偏氟乙烯（Polyvinylidene Fluoride, PVDF）作为锂离子电池石墨基负极黏结剂，得到广泛应用。但是，PVDF用作硅基负极黏结剂时，因其对硅颗粒的黏附力较弱，无法保持硅基负极的稳定循环，而且在硅基材料的体积膨胀过程中不能保持电极的完整性[19-20]。为了开发出有效的硅基负极用黏结剂，探索了多种功能聚合物材料的应用，主要有高弹性聚合物黏结剂、自修复聚合物黏结剂和导电聚合物黏结剂，如图1所示[21]。本文综述近年来硅基负极用黏结剂的研究进展，旨在为硅基负极用黏结剂的开发和应用提供建议。
1 高弹性聚合物黏结剂
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高弹性黏合剂，通常是通过聚合物分子的结构优化或增加配位键和共价键的含量来制备。高弹性黏合剂具有较高的杨氏模量，可以缓解硅基电极材料循环期间的体积变化，而使黏结剂不会发生失效[22]。传统的聚丙烯酸（Polyacrylic Acid, PAA）、丁苯橡胶（Styrene Butadiene Rubber, SBR）等聚合物黏结剂，具有很强的分子间相互作用，但是该类黏结剂通过低含量的羧酸盐基团，以及与硅颗粒的点或线接触，降低了它们的黏结强度。为此，合成设计新型黏结剂材料、对传统黏结剂材料实施改性[23-24]。
Tang等[25]在羧甲基纤维素（Carboxymethyl Cellulose, CMC）中加入聚多巴胺（Polydopamine, PDA），并在此基础上开发了CMC/PDA复合黏结剂，该黏结剂表现出优异的黏结力，达到10.8 N。同时，复合黏结剂中CMC和PDA通过氢键互相连接，如图2所示。拉伸率高达128.7%。将此复合黏结剂应用于硅基负极锂离子电池，活性材料和金属集流体之间具有更好的黏结性，而高的拉伸性有利于缓冲硅颗粒体积增大变化。优异的机械性能有助于保持电极的完整性和多孔结构，从而在循环过程中稳定电池容量。在0.2 C的电流密度下，使用复合黏合剂的锂离子电池，在150次循环后具有80%的高容量保持率，首次库伦效率高达87%。此外，Zhang等[26]制备了PAA/PDA复合黏结剂，应用于硅基负极锂离子电池，黏接强度提高了100%以上。电池循环性能也得到显著提高，100次循环后容量保持率为77.7%，200次循环后容量保持率为68.1%。
Luo等[27]通过原子转移自由基聚合制备了多臂PAA（4A-PAA），并应用于黏结剂。结果发现，与传统的线性PAA黏结剂相比，4A-PAA不仅由于其分子内氢键而显示出增强的韧性，而且由于其多维结构而显示出显著的结合强度。通过力学试验发现，4A-PAA黏结剂在断裂前可以承受3.3%的应变，而PAA黏结剂只能承受1.4%的应变。此外，4A-PAA黏结剂表现出更高的断裂强度，约为PAA的1.6倍。将其应用于硅基负极锂离子电池，由于4A-PAA黏结剂有助于减轻硅基负极循环期间的体积变化，因此电池表现出优异的循环性能。在电流密度为0.16 A·g-1、循环200次后，电池仍具有89.1%的容量保持率和558.1 mA·h/g的容量，相对于使用PAA黏结剂的锂离子电池，使用4A-PAA黏剂电池容量提高了10%以上。
Zhao等[28]将壳聚糖（Chitosan, CS）用作锂离子电池硅基负极黏结剂，电池表现出稳定的循环性能，CS结构式如图3所示。除此之外，将CS与醋酸或PAA混合，由于CS的-NH2基团与羧酸的-COOH基团之间发生交联反应，形成聚合物网状结构（图4），能够有效地适应了硅颗粒在循环过程中的体积变化，从而实现了电池的高库仑效率和优异的循环性能。此外，木质素[29]、聚乙烯-丙烯酸乙酯-马来酸酐共聚热塑性弹性体[30]、海藻酸钠[31]、天然胶[32]也相继被应用于硅基负极黏结剂，取得较好效果。
关于高弹性聚合物黏结剂的开发，一般通过改性的方式引入大量羧基，增加了与硅基负极表面羟基相互作用形成氢键的数量，可以承受硅基负极体积变化，有效保持电极的机械完整性。而且为了进一步提高黏结强度，通过分子结构设计将三维网状聚合物应用于高弹性聚合物黏结剂，逐渐成为研究热点，如酯化反应、原位交联聚合等。
2 自修复聚合物黏结剂
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自修复概念，来源于人体骨骼或皮肤等可以自动愈合的生物系统。自修复聚合物（Self-Healing Polymer, SHP）是一种无需任何外部干预即可自动修复内部裂缝或损伤的材料。自修复聚合物的自修复机制主要有2种：
（1）利用预埋的自修复剂，促进损伤区域的分子片段流动，达到修复效果；
（2）无需自修复剂，通过共价键、自由基键或超分子动态键结合，达到修复效果[33-35]。
在锂离子电池循环过程中，硅基负极不断膨胀，硅材料和黏结剂容易断裂，进一步降低循环性能。采用具有自修复特性的黏结剂，可以再生其原始结构并改变电极和集电器之间的界面力，如图5所示[9,36]。
Zhang等[37]将脲基嘧啶酮单体（Ureidopyrimidinone, UPy）与线性PAA共价结合，得到一种自修复超分子聚合物PAA-UPy，用于锂离子电池硅基负极黏结剂。由于其四重氢键动态相互作用，所获得的聚合物被证明具有优异的自愈能力。这种超分子黏结剂与硅颗粒之间具有强的结合力，可有效承受锂化和脱锂时，硅基负极大的体积变化。使用这种自修复超分子聚合物作为黏结剂的电池，初始放电容量高达4 194 mA·h/g和库伦效率为86.4%，优于使用PAA、CMC和PVDF黏结剂的电池。此外，在110次循环后仍保持有2 638 mA·h/g的高容量，显示出良好的长期循环稳定性。
Munaoka等[38]首先合成了SHP，并引入了聚乙二醇（Polyethylene Glycol, PEG）基团，得到SHP-PEG，其结构示意如图6所示。同时用该聚合物SHP-PEG制备了硅基负极黏结剂，SHP-PEG黏结剂中的尿素氢键对硅颗粒表面产生有效的附着力和循环后裂纹的自修复。因此，即使在循环后硅颗粒发生破损后，电极结构也具有机械性能和电化学性能的保持能力。SHP-PEG中的PEG基团可以减轻硅颗粒和电解质之间的电荷转移阻力，起到促进锂离子传导以实现良好的倍率性能的作用。Nam等[39]在上述基础上，基于含有UPy官能团的PAA聚合物，通过接枝引入PEG，命名为PAU-g-PEG，并应用于锂离子电池硅基负极黏结剂，也发现类似现象。
目前，制备自修复聚合物黏结剂一般通过形成动态三维网状结构来实现。天然高分子材料（如CMC、CS、木质素）具有来源广、易于制备、环境友好的优点，而且分子链含有大量的羧基、羟基、氨基官能团，因此基于天然高分子材料的自修复聚合物黏结剂成为研究热点。
3 导电聚合物黏结剂
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硅用于锂离子电池的负极材料时，由于硅的固有电导率低，通常需要制备硅和碳复合电极材料和增加导电添加剂来提高整个电极电导率。常用的碳基导电添加剂是非黏性的，在硅的连续体积变化过程中容易与硅颗粒断开。而且传统黏结剂和导电添加剂都具有电化学惰性，对电池能量密度提升没有任何贡献。使用导电聚合物作为黏结剂和导电添加剂有望整体提高电极导电性，同时通过增加电极中活性材料的比例来提高电池能量密度[40-42]。
Zhu等[43]合成了导电聚合物聚（9,9-二辛基芴-芴酮-苯甲酸甲酯）（PFM），并将其用于锂离子电池的硅基负极黏结剂，其结构式如图7所示。由于PFM黏结剂具有出色的机械应力耐受性、黏结性能和导电性，因此电池表现出优异的循环性能，经过100次循环之后，电池仍具有超过99.5%的库伦效率。而且使用PFM黏结剂的电池，20次电池循环之后，电池未出现容量衰减。而使用PVDF黏结剂的电池，10次电池循环之后，就出现容量衰减和早期的电池故障。基于以上分析，PFM黏结剂具有良好的硅颗粒附着力和表面保护效果。
Chen等[44]以过硫酸铵（Ammonium Persulfate, APS）为氧化剂，将苯胺（Aniline, AN）与聚苯乙烯磺酸（Polystyrene Sulfonic Acid, PSSA）发生直接化学氧化物聚合反应合成PSSA@PANI聚合物（图8），并将该聚合物与聚乙烯醇（Polyvinyl Alcohol, PVA）共混制备出水溶性导电聚合物复合材料，将其用于硅基负极黏结剂。由于其具有导电和水溶性的性质，这些聚合物复合材料表现出优异的黏结剂性能。由于其具有导电和水溶性的特点，该聚合物复合材料表现出优异的黏结性能。由于该黏结剂与硅颗粒之间独特的相互作用，以及具有导电的PSSA@PANI骨架，可以缓冲锂化过程中硅的体积膨胀并促进电荷转移。因此，使用该复合黏合剂制备的硅基负极锂离子电池，表现出优异的锂存储可逆性和循环稳定性。
Tang等[45]采用PVA、聚3,4-乙烯二氧噻吩∶聚苯乙烯磺酸（PEDOT: PSS）和PDA，制备了三元聚合物黏结剂，其工作机理见图9。PEDOT: PSS具有优良的导电性，可以提高硅负极导电性。而PVA和PDA具有较高的键合能力，极大地增强硅材料和集流体之间的附着力，从而可以提高锂离子电池的循环稳定性。此外，PVA复合后可以显著提高黏结剂的柔韧性，从而适应硅的体积变化，提高硅基负极的电池循环稳定性。
作为一种特殊聚合物，具有电子导电性的共轭聚合物，可以用作硅基负极中的黏结剂和导电添加剂，具有研究前景。PF基、PANI基和PEDOT: PSS基是目前研究热度最高的导电聚合物黏结剂。
为了开发出有效的硅基负极黏结剂，实现基于硅基负极的锂离子电池应用，新型聚合物逐渐用于黏结剂应用研究。而且，除了单一类型的聚合物黏结剂，还可以通过聚合物改性，使黏结剂兼具各种功能，从而实现黏结剂的多功能化。Su等[46]将导电聚合物PEDOT: PSS和聚醚硫脲（Poly Ether-Thioureas, PETU）交联制备了多功能聚合物黏结剂，兼具导电性和高弹性。Zeng等[47]将离子聚合物聚环氧乙烷和聚乙烯亚胺引入到PEDOT: PSS分子链，所制得的聚合物黏结剂，具有高离子电导率和电子导电性。
表1总结了本文综述的近年来不同种类黏结剂，及其在硅基负极锂离子电池中的电化学表现，可以看出新型聚合物黏结剂电池性能均优于PVDF黏结剂电池性能。同时也可以发现具有交联网状结构的聚合物黏结剂，如CS-g-PAAA、OS-CMC、PSSA@PANI，表现出更高的首次放电比容量和更优的循环稳定性。
4 结束语
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锂离子电池在新能源汽车产业中至关重要，黏结剂虽然在锂离子电池中的用量很少，但是黏结剂对于保持锂离子电池的电极完整性和稳定性方面发挥着关键作用。由于硅基负极材料在锂化过程中，发生很大体积膨胀和由此导致的严重容量退化，聚合物黏结剂在减小体积膨胀和保持硅基负极的机械和电化学完整性方面，发挥着关键作用。为了促进锂离子电池硅基负极材料的实际应用，开发了不同结构、性质、功能的聚合物黏结剂。
当前，锂离子电池硅基负极应用最多的黏结剂仍然是CMC/SBR黏结剂。开发新型聚合物黏结剂，有效缓解硅基负极的体积膨胀，促进高容量硅基负极材料在高能量密度锂离子电池中的大规模应用，仍需要广大科技工作者进一步发挥创新力。
（1）现有新开发的黏结剂结构较为复杂，工艺流程较为繁多，不利于工业生产和成本控制，因此需要简化合成程序，降低新型黏结剂成本。
（2）结合聚合物材料改性方式，探索多功能聚合物黏结剂，满足不同应用需求。鉴于计算技术的快速发展，可以基于人工智能和机器学习技术，开展聚合物黏结剂配方的快速筛选和结构优化。
（3）现有硅基负极黏结剂的电化学评价方式，一般采用半电池的形式，但是半电池一般含有大量的电解质，很难有效反映黏结剂在硅基负极中的实际作用。因此，采用商业全电池模式甚至极端条件下的评价，有利于硅基负极黏结剂设计和开发的实用性。
相信随着材料科学、理论研究的深入、工艺水平和研发能力的提高，聚合物黏结剂能够克服诸多不利因素，满足锂离子电池硅基负极更高的性能和品质要求，助力新能源汽车行业发展与升级。
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2023年第卷第8期
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doi: 10.19822/j.cnki.1671-6329.20220177
  • 首发时间：2026-01-04
  • 出版时间：2023-08-05
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鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
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