锂离子电池硅基负极用功能粘结剂的研究进展

doi:10.3866/PKU.WHXB202306006

物理化学学报 >> 2024, Vol. 40 >> Issue (6): 2306006.doi: 10.3866/PKU.WHXB202306006

锂离子电池硅基负极用功能粘结剂的研究进展

张景硕¹, 翟越¹, 赵子云¹, 何家兴¹, 魏伟³, 肖菁¹^,³^,⁴, 吴士超¹^,²^,*, 杨全红¹^,²^,³^,⁴^,*

¹ 天津大学化工学院Nanoyang课题组, 国家储能产学研一体化平台, 天津化学化工协同创新中心, 天津市先进碳与电化学储能重点实验室, 天津 300072
² 物质绿色创造与制造海河实验室, 天津 300192
³ 天目湖先进储能技术研究院, 江苏溧阳 213300
⁴ 天津大学-新加坡国立大学福州联合学院, 天津大学福州国际研究院, 福州 350207

收稿日期:2023-06-02 修回日期:2023-07-05 录用日期:2023-07-20 发布日期:2023-11-29
通讯作者: Email: wushichao@tju.edu.cn (吴士超)qhyangcn@tju.edu.cn (杨全红)
基金资助:
国家重点研究发展计划(2021YFF0500600); 国家自然科学基金(U2001220); 国家自然科学基金(52272231)

Research Progress of Functional Binders in Silicon-Based Anodes for Lithium-Ion Batteries

Jingshuo Zhang¹, Yue Zhai¹, Ziyun Zhao¹, Jiaxing He¹, Wei Wei³, Jing Xiao¹^,³^,⁴, Shichao Wu¹^,²^,*, Quan-Hong Yang¹^,²^,³^,⁴^,*

¹ Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), and National Industry-Education Integration Platform of Energy Storage, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
² Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China
³ Tianmu Lake Institute of Advanced Energy Storage Technologies, Liyang 213300, Jiangsu Province, China
⁴ Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, China

Received:2023-06-02 Revised:2023-07-05 Accepted:2023-07-20 Published:2023-11-29
Contact: Email: wushichao@tju.edu.cn (Shichao Wu)qhyangcn@tju.edu.cn (Quan-Hong Yang)
Supported by:
the National Key Research and Development Program of China(2021YFF0500600); the National Natural Science Foundation of China(U2001220); the National Natural Science Foundation of China(52272231)

摘要/Abstract

摘要：

硅(Si)具有超高的理论比容量、较低的嵌锂电位及丰富的储量等优势，是发展高比能锂离子电池的关键负极材料。同纳米Si相比，低成本、高振实密度和低界面反应的微米Si应用于高体积能量密度器件独具优势。然而其300%体积形变产生的巨大应力，使得颗粒破碎粉化、电极结构退化以及导电网络失效等问题更为严峻，极大制约了其商业化进程。粘结剂是适应Si体积变化，提供稳定导电网络的重要手段。开发高容量、高稳定微米Si基负极对粘结体系设计提出了更大的挑战。本文首先阐明了粘结剂的基础功能与粘结机制，然后从自愈合、电子导电、离子导电以及参与固态电解质层构建四个方面，总结了Si基负极用功能粘结剂的设计策略和作用原理，最后展望了面向实用化的Si基负极功能粘结剂面临的挑战和未来发展方向。

关键词: 锂离子电池, 硅基负极, 功能粘结剂, 自愈合聚合物, 导电聚合物

Abstract:

Silicon (Si) has a high theoretical gravimetric capacity (3579 mAh∙g⁻¹ for Li₁₅Si₄), which is almost ten times higher than that of graphite (372 mAh∙g⁻¹) anode. Besides, it has low electrochemical potentials (0.4 V vs. Li⁺/Li), and abundant reserves. Thus, Si becomes a key anode material for the development of high-energy lithium-ion batteries. Nano-Si, typically compounded with graphite, has opened its commercialization. But the specific capacity of commercial Si/graphite composites is generally below 600 mAh∙g⁻¹, which is far below the theoretical specific capacity of Si. In the meanwhile, the high cost, high specific surface area and low tap density of nano-Si limit its volumetric energy density and large-scale production further. Compared to the above materials, micro-Si (1–10 μm) is gaining industry attention for its low cost, as it does not require high-energy ball milling to reduce the particle size. Also, low specific surface area and high tap density conduce to reducing interfacial side reactions and increasing volumetric energy density. Therefore, micro-Si has a particular advantage over application in high volumetric energy density storage devices. However, due to the huge stress caused by significant volume change (300%), there are more severe problems such as particle pulverization, electrode disintegration, conductive network failure and uncontrolled growth of solid electrolyte interphases, which greatly hinder its commercialization. Binders are essential in adapting to Si volume changes to ensure the integrity of the electrode and keeping the tight contact among the active material, conductive additive and current collector to provide a stable conductive network. The development of high-capacity and high-stability micro-Si-based anodes poses greater challenges to the design of binders. In this review, we first clarify the binding mechanism of binders, factors that influence the bonding forces, and design strategies of binders for relieving the volume change of Si electrodes. As a major part, we systematically discuss the strategies and corresponding mechanisms of functional binders for silicon-based anodes from aspects of self-healing binders, conductive binders, ion-conductive binders, and the facilitating effect of functional binders on the stable SEI (Solid Electrolyte Interphase) formation. Finally, the existing problems and challenges are pointed out in terms of long-cycle stability, initial Coulombic efficiency (ICE) and binder ratio under commercial loading. We put forward the promising directions for developing functional binders towards the practical use of micro-Si anode: an ideal binder should be multifunctional and helpful to robust electron/ion conductive networks and stable SEI throughout the long cycling life of micro-Si, where the polymer molecular structure of functional binders can be systematically designed by artificial intelligence and machine learning technologies.

Key words: Lithium-ion battery, Silicon-based anode, Functional binder, Self-healing polymer, Conductive polymer

张景硕, 翟越, 赵子云, 何家兴, 魏伟, 肖菁, 吴士超, 杨全红. 锂离子电池硅基负极用功能粘结剂的研究进展[J]. 物理化学学报, 2024, 40(6), 2306006. doi: 10.3866/PKU.WHXB202306006

Jingshuo Zhang, Yue Zhai, Ziyun Zhao, Jiaxing He, Wei Wei, Jing Xiao, Shichao Wu, Quan-Hong Yang. Research Progress of Functional Binders in Silicon-Based Anodes for Lithium-Ion Batteries[J]. Acta Phys. -Chim. Sin. 2024, 40(6), 2306006. doi: 10.3866/PKU.WHXB202306006

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202306006

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I6/2306006

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表1

功能粘结剂电化学性能总结"

Binder	Binder ratio	Areal capacity (mAh∙cm⁻²)	First discharge capacity (mAh∙g⁻¹)	ICE	Capacity retention	Rate performance (mAh∙g⁻¹)
PR-PAA	10%	2.67@0.64 mA∙cm⁻²	2971@0.1 A∙g⁻¹	91.2%	91%@150 cycles	1400@3 A∙g⁻¹
PAA-P(HEA-co-DMA)	10%	3.2@1 A∙g⁻¹	2850@0.4 A∙g⁻¹	89.3%	94%@220 cycles	1855@5 A∙g⁻¹
SHP	50%	2.1@0.2 A∙g⁻¹	3400@0.4 A∙g⁻¹*	78%*	80%@90 cycles	1400@2 A∙g⁻¹
3D SHP	33%	3.8@0.3 mA∙cm⁻² *	2620@0.42 A∙g⁻¹	92.0%	70%@140 cycles	–
SBR/CMC-PEG-Im-Zn²⁺	10%	2@0.65 A∙g⁻¹ *	640@0.65 A∙g⁻¹	–	100%@200 cycles *	261@1.3 A∙g⁻¹
PAA-BFPU	15%	3@0.8 A∙g⁻¹ *	3500@0.2 A∙g⁻¹	89.8%	86%@100 cycles	1309@6 A∙g⁻¹
SHPET	20%	3.6@0.84 A∙g⁻¹ *	3744@0.42 A∙g⁻¹	86.0%	63%@60 cycles *	1594@4.2 A∙g⁻¹
GCA	15%	3.6@2 A∙g⁻¹	4015@0.2 A∙g⁻¹	89%*	72%@100 cycles	2416@4 A∙g⁻¹
PAA-UPy	20%	2.1@0.84 A∙g⁻¹ *	4194@0.84 A∙g⁻¹	86.4%	74%@110 cycles	2662@21 A∙g⁻¹ discharge, 0.84 A∙g⁻¹ charge
DA-PAA	30%	1.4@0.42 A∙g⁻¹ *	2607@0.42 A∙g⁻¹	86.0%	48%@200 cycles *	2190@21 A∙g⁻¹
AXDY-PA	20%	2.5@0.5 A∙g⁻¹ *	4113@0.5 A∙g⁻¹	87.0%	75%@100 cycles	1446@8 A∙g⁻¹
GCS-OSA	20%	2.8@0.84 A∙g⁻¹ *	4581@0.84 A∙g⁻¹	77.1%	43%@200 cycles *	2185@21 A∙g⁻¹
PAA-DA/PVA	20%	–	3434.3@0.4 A∙g⁻¹	83.4%	73%@100 cycles	2168@4 A∙g⁻¹
PEFM	33%	0.6@0.092 mAh∙cm⁻² *	3750@0.092 mAh∙cm⁻²	70.0%	84%@50 cycles	2730@1.84 mAh∙cm⁻²
PF-COONa	33%	1.5@0.42 A∙g⁻¹ *	3500@0.42 A∙g⁻¹	68.4%	84%@100 cycles	1424@8.4 A∙g⁻¹
PEDOT: PSS-FA	20%	3.8@0.5 A∙g⁻¹	3685@0.5 A∙g⁻¹	77.5%	63%@100 cycles *	1550@5 A∙g⁻¹
PEDOT: PSS-GOPS	27.30%	2.9@1 A∙g⁻¹	3450@1 A∙g⁻¹	85.0%	70.8%@200 cycles	760@8 A∙g⁻¹
PPTU	20%	2@1 A∙g⁻¹ *	3950@0.2 A∙g⁻¹	80.1%	76.7%@300 cycles	620@8 A∙g⁻¹
Polyimine	5%	1.3@0.4 A∙g⁻¹ *	–	60.0%	80.4%@200 cycles	433@5 A∙g⁻¹
PVA-CS-CPDs	10%	5.4@0.42 A∙g⁻¹ *	3048@0.84 A∙g⁻¹	89.6%	60%@100 cycles *	1076@8.4 A∙g⁻¹
CG	10%	6.4@0.3 mA∙cm^{−2 *}	3788	80.0%	80%@300 cycles *	737@8.4 A∙g⁻¹
GG	15%	2.8@0.84 A∙g⁻¹ *	3364@2.1 A∙g⁻¹	88.3%	70%@30 cycles	980@12.6 A∙g⁻¹
N-P-LiPN	10%	5@0.84 A∙g⁻¹ *	3650@0.84 A∙g⁻¹	86.2%	70%@50 cycles *	2021@8.4 A∙g⁻¹
xPEG-GCS	20%	1.4@0.36 A∙g⁻¹	3332@0.36 A∙g⁻¹	82.2%	64.7%@150 cycles	2700@10.74 A∙g⁻¹
c-PEO-PEDOT: PSS/PEI	20%	~4@1 A∙g⁻¹	2440@1 A∙g⁻¹	82.0%	~100%@60cycles	1590@8 A∙g⁻¹
SHP-PEG	30%	1.1@1.79 A∙g⁻¹	2600@0.179 A∙g⁻¹	83.0%	80%@150 cycles	900@7.16 A∙g⁻¹
GG-g-PAM	5%	5.1@0.5 A∙g⁻¹	2600@0.15 A∙g⁻¹	84.5%	78.5%@60cycles	1249@8 A∙g⁻¹

表1

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Research Progress of Functional Binders in Silicon-Based Anodes for Lithium-Ion Batteries

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