Role of Polyacrylic Acid (PAA) Binder on the Solid Electrolyte Interphase in Silicon Anodes

聚丙烯酸 电解质 阳极 化学工程 材料科学 X射线光电子能谱 锂(药物) 离子液体 电极 化学 复合材料 聚合物 有机化学 光电子学 医学 工程类 内分泌学 物理化学 催化作用
作者
Pritesh Parikh,Mahsa Sina,Abhik Banerjee,Xuefeng Wang,Macwin Savio D’Souza,Jean‐Marie Doux,Erik A. Wu,Osman Y. Trieu,Yongbai Gong,Qian Zhou,Kent Snyder,Ying Shirley Meng
出处
期刊:Chemistry of Materials [American Chemical Society]
卷期号:31 (7): 2535-2544 被引量:183
标识
DOI:10.1021/acs.chemmater.8b05020
摘要

To obtain high-energy density Li-ion batteries for the next-generation storage devices, silicon anodes provide a viable option because of their high theoretical capacity, low operating potential versus lithium (Li), and environmental abundance. However, the silicon electrode suffers from large volume expansion (∼300%) that leads to mechanical failure, cracks in the SEI (solid electrolyte interphase), and loss of contact with the current collector, all of which severely impede the capacity retention. In this respect, the choice of binders, carbon, electrolyte, and the morphology of the silicon itself plays a critical role in improving capacity retention. Of specific mention is the role of binders where a carboxylic acid-heavy group, PAA (polyacrylic acid), has been demonstrated to have better cycling capacity retention as compared to CMC (carboxy methyl cellulose). Traditionally, the role of binders has been proposed as a soft matrix backbone that allows volume expansion of the anode while preserving its morphology. However, the effect of the binder on both the rate of formation of SEI species across cycles and its distribution around the silicon nanoparticles has not been completely investigated. Herein, we use two different binders (PAA and CMC) coupled with LiFSI (lithium bis(fluorosulfonyl)imide)/EMI-FSI (1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide) ionic liquid as the electrolyte to understand the effect of binder on the SEI. Using STEM-EDX (scanning transmission electron microscopy–energy-dispersive X-ray spectroscopy), EELS (electron energy loss spectroscopy), and XPS (X-ray photoelectron spectroscopy), we discuss the evolution of the SEI on the Si electrode for both binders. Our results indicate that a faster decomposition of FSI– with a PAA binder leads to LiF (lithium fluoride) formation, making F– unavailable for subsequent SEI formation cycles. This allows further decomposition of the LiFSI salt to sulfates and sulfides which form a crucial component of the SEI around silicon nanoparticles after 100 cycles in the PAA binder-based system. The dual effects of faster consumption of F– to form LiF together with the distribution of passivating sulfides in the SEI could allow for better capacity retention in the PAA binder system as compared to that with CMC.
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