Graduate School of Energy, Environment, Water and Sustainability (EEWS), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.
School of Chemical and Biological Engineering and Institute of Chemical Processes, Seoul National University, 1 Gwanak-ro Gwanak-gu, Seoul 08826, Republic of Korea.
Chem Soc Rev. 2018 Mar 21;47(6):2145-2164. doi: 10.1039/c7cs00858a. Epub 2018 Feb 7.
Silicon (Si) anode is among the most promising candidates for the next-generation high-capacity electrodes in Li-ion batteries owing to its unparalleled theoretical capacity (4200 mA h g for LiSi) that is approximately 10 times higher than that of commercialized graphitic anodes (372 mA h g for LiC). The battery community has witnessed substantial advances in research on new polymeric binders for silicon anodes mainly due to the shortcomings of conventional binders such as polyvinylidene difluoride (PVDF) to address problems caused by the massive volume change of Si (300%) upon (de)lithiation. Unlike conventional battery electrodes, polymeric binders have been shown to play an active role in silicon anodes to alleviate various capacity decay pathways. While the initial focus in binder research was primarily to maintain the electrode morphology, it has been recently shown that polymeric binders can in fact help to stabilize cracked Si microparticles along with the solid-electrolyte-interphase (SEI) layer, thus substantially improving the electrochemical performance. In this review article, we aim to provide an in-depth analysis and molecular-level design principles of polymeric binders for silicon anodes in terms of their chemical structure, superstructure, and supramolecular interactions to achieve good electrochemical performance. We further highlight that supramolecular chemistry offers practical tools to address challenging problems associated with emerging electrode materials in rechargeable batteries.
硅（Si）阳极由于其无与伦比的理论容量（LiSi 的 4200 mA h g-1），大约是商业化石墨阳极（LiC 的 372 mA h g-1）的 10 倍，是下一代高容量锂离子电池中最有前途的候选者之一。由于传统粘结剂（如聚偏二氟乙烯（PVDF））存在一些缺点，例如无法解决硅（300%）在（脱）锂过程中体积变化过大的问题，因此电池界在硅阳极用新型聚合物粘结剂的研究方面取得了实质性进展。与传统电池电极不同，聚合物粘结剂已被证明在硅阳极中发挥积极作用，可以缓解各种容量衰减途径。虽然粘结剂研究的最初重点主要是维持电极形态，但最近已经表明，聚合物粘结剂实际上可以帮助稳定开裂的硅微颗粒以及固体电解质界面（SEI）层，从而显著提高电化学性能。在这篇综述文章中，我们旨在从化学结构、超结构和超分子相互作用的角度深入分析和分子水平设计用于硅阳极的聚合物粘结剂，以实现良好的电化学性能。我们进一步强调，超分子化学提供了实用工具，可以解决与可再充电电池中新兴电极材料相关的具有挑战性的问题。
