As opposed to nano‐Si anodes, Si‐microparticle (Si‐MP)‐based negative electrode is still in an immature stage due to the fragility of particles of which dimension is farther from the critical size of Si. In terms of binder chemistry, the established strategies for nano‐Si anode can be moderately transferred to designing functional binders for commercially available Si‐MP. However, only a few studies have reported acceptable electrochemical properties of Si‐MP in the level of designing novel‐binder systems. Herein, the ionically crosslinked polyacrylate (PANa_0.8Fe_y) inspired by metallo‐supramolecular polymers is introduced as a binder for Si‐MP anode. Although cracking of Si‐MP is inevitable during cycles, the electrode components can effectively be confined within the supramolecular network, which reversibly adjusts its architecture via iron (Fe³⁺)‐carboxylate coordination. With appropriate compositions, the incorporation of ferric ion to sodium polyacrylate allows the Si‐MP to exhibit an excellent round‐trip capacity of ∼1400 mAh g⁻¹ after 400 cycles. The resulting electrochemical performance is demonstrated by several correlated factors: (i) type of supramolecular interactions, (ii) effect of cations (Na⁺/Fe³⁺) on the conformation of polymer, and (iii) mechanical properties of the electrode.

中文翻译：

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金属配位介导的聚丙烯酸酯，用于高性能硅微粒阳极

与纳米Si阳极相反，基于Si微粒（Si-MP）的负极仍处于不成熟阶段，这是因为其尺寸远小于Si的临界尺寸的颗粒易碎。在粘合剂化学方面，可以将已建立的纳米Si阳极策略适当地转移到设计用于商用Si-MP的功能粘合剂。然而，只有很少的研究报道了在新型粘合剂体系设计水平上可接受的Si-MP电化学性能。在此，离子交联聚丙烯酸酯（PANa _0.8 Fe _y引入了金属超分子聚合物作为Si-MP阳极的粘结剂。尽管在周期内不可避免地会发生Si-MP的开裂，但电极成分可以有效地限制在超分子网络内，这可通过铁（Fe ³⁺）-羧酸盐配位可逆地调整其结构。通过适当的组成，在聚丙烯酸钠中掺入铁离子可使Si-MP在400次循环后展现出约1400 mAh g ^-1的出色往返容量。几个相关因素证明了所得的电化学性能：（i）超分子相互作用的类型，（ii）阳离子（Na ⁺ / Fe ³⁺）关于聚合物的构造，以及（iii）电极的机械性能。