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Room-Temperature Crosslinkable Natural Polymer Binder for High-Rate and Stable Silicon Anodes

机译：适用于高速率和稳定硅阳极的室温可交联天然聚合物粘合剂

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摘要

Natural polymers with abundant side functionalities are emerging as a promising binder for high-capacity yet large-volume-change silicon anodes with a strong and reversible supramolecular interaction that originates from secondary bonding. However, the supramolecular network solely based on hydrogen bonding is relatively vulnerable to repeated deformation and has an insufficient diffusivity of lithium ions. Herein, reported is a facile but efficient way of incorporating the natural polymers with an ionically conductive crosslinker, which can construct a robust network for silicon anodes. The boronic acid in the crosslinker spontaneously reacts with natural polymers to generate boronic esters at room temperature without any kind of triggers, which gives a strong and dynamic covalent bonding to the supramolecular network. The other component in the crosslinker, polyethylene oxide, contributes to the enhanced ionic conductivity of polymers, leading to outstanding rate performances even at a high mass loading of silicon nanoparticles (>2 mg cm(-2)). The small portion of the proposed crosslinker can modulate the strength of the entire network by balancing the covalent crosslinking and self-healing secondary interaction along with the fast lithium-ion diffusion, thus enabling the extended operation of silicon electrodes.
机译：具有丰富的侧链功能的天然聚合物正成为一种有前途的粘合剂，可用于大容量，大体积变化的硅阳极，这种阳极具有强大且可逆的超分子相互作用，这种相互作用源自二次键合。然而，仅基于氢键的超分子网络相对容易重复变形，并且锂离子的扩散性不足。本文中，报道了一种将天然聚合物与离子导电交联剂结合的简便但有效的方法，其可为硅阳极构建坚固的网络。交联剂中的硼酸在室温下与天然聚合物自发反应，生成硼酸酯，而没有任何类型的触发因素，从而使超分子网络具有牢固而动态的共价键合。交联剂中的另一种成分，聚环氧乙烷，有助于提高聚合物的离子电导率，即使在硅纳米颗粒的高质量负载（> 2 mg cm（-2））下，也具有出色的速率性能。所提出的交联剂的一小部分可以通过平衡共价交联和自我修复的二次相互作用以及快速的锂离子扩散来调节整个网络的强度，从而使硅电极的操作得以扩展。

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