The major cause for capacity fading of silicon nanoparticle (SiNP)-based electrodes is the immense pressure applied toward the conductive networks during the charge/discharge process. While numerous efforts have been devoted to investigating different types of polymer binders, the rational design of an adhesive binder with pressure sensitivity has rarely been reported. Herein, a series of pressure-sensitive adhesives (PSAs) synthesized via copolymerization of 2-ethylhexyl acrylate (2-EHA) and acrylic acid (AA) are evaluated as polymer binders for SiNP-based electrodes. The balance between the density of interaction groups and viscoelastic properties is systematically investigated for efficient binding performance. The SiNP-based electrode using PSA with 20 mol % of 2-EHA (Si-PSA-20%) exhibits excellent electrochemical performance, achieving a capacity retention of 83% at the 100th cycle compared with 54% for Si-PAA after activation. Si-PSA-20% also delivers a superior cycling performance at a high current density (1731 mAh g^–1 after 350 cycles vs 719 mAh g^–1 after 150 cycles for Si-PAA, 1.8 A g^–1) and at high mass loading of active materials (capacity retention of 74 vs 38% for Si-PAA after 100 cycles, SiNP content ∼1.2 mg cm^–2). Atomic force microscopy (AFM), peel tests, and Car–Parrinello molecular dynamics (CPMD) simulations are employed to understand their binder performance. The novel design and systematical investigation of PSAs as binders will definitely be appealing for not only the Si electrode but also for other high-energy-density electrode materials.

中文翻译：

---

胶粘剂聚合物作为高容量硅电极的高效粘合剂

硅纳米粒子（SiNP）基电极的容量衰减的主要原因是在充电/放电过程中施加给导电网络的巨大压力。尽管已致力于研究不同类型的聚合物粘合剂的大量努力，但很少报道具有压力敏感性的粘合剂粘合剂的合理设计。在此，评估了通过丙烯酸2-乙基己酯（2-EHA）和丙烯酸（AA）的共聚合成的一系列压敏粘合剂（PSA）作为用于SiNP基电极的聚合物粘合剂。为了有效的结合性能，系统地研究了相互作用基团的密度和粘弹性之间的平衡。使用PSA与20 mol％的2-EHA（Si-PSA-20％）的SiNP基电极表现出出色的电化学性能，激活后第100个循环的容量保持率为83％，而Si-PAA为54％。Si-PSA-20％在高电流密度（1731 mAh g^-1后350次循环VS 719毫安克^-1后150个循环的Si-PAA，1.8 A G ^-1），并在活性物质的高质量负载（74和38％的容量保持率对硅-PAA 100个循环，之后SINP含量〜1.2 mg cm ^–2）。原子力显微镜（AFM），剥离测试和Car-Parrinello分子动力学（CPMD）模拟被用来了解其粘合剂性能。PSA作为粘合剂的新颖设计和系统研究无疑将不仅对Si电极而且对其他高能量密度电极材料也具有吸引力。