Silicon has been regarded as one of the most promising anodes for lithium-ion batteries (LIBs). However, state-of-the-art silicon-based material suffers from huge volume changes and poor conductivity. Here, we develop a surface engineering strategy to address the intrinsic defects. A dual-binder formed by cross-linking sodium alginate and chitosan is investigated and proposed. Moreover, a 3,4,9,10-perylenetetracarboxylic diimide (PDI) shell is introduced into the Si@SiO_x surface. Density functional theory (DFT) calculations reveal that π-π stacking PDI with Li-ion trapping properties is compatible with an SA/CS complex (SC) binder through strong adsorption. These factors buffer the interface tension of Si@SiO_x and facilitate Li-ion diffusion. The fabricated electrode shows highly reversible lithium-ion storage and long-term stability. Furthermore, a full-cell configuration with lithium nickel cobalt manganate (NCM) as the cathode demonstrates superior electrochemical properties and potential applications. Such surface engineering creates an opportunity for the fabrication of advanced silicon anodes.

硅一直被认为是最有前途的锂离子电池（LIBs）负极之一。然而，最先进的硅基材料存在巨大的体积变化和较差的导电性。在这里，我们开发了一种表面工程策略来解决固有缺陷。研究并提出了由海藻酸钠和壳聚糖交联形成的双粘合剂。此外，3,4,9,10-苝四羧酸二酰亚胺（PDI）壳被引入到Si@SiO _x表面。密度泛函理论 (DFT) 计算表明，具有锂离子捕获特性的 π-π 堆积 PDI 通过强吸附与 SA/CS 复合物 (SC) 粘合剂兼容。这些因素缓冲了 Si@SiO _x的界面张力并促进锂离子扩散。制造的电极显示出高度可逆的锂离子存储和长期稳定性。此外，以镍钴锰酸锂（NCM）为阴极的全电池配置显示出优异的电化学性能和潜在应用。这种表面工程为制造先进的硅阳极创造了机会。