Adhesive Polymers as Efficient Binders for High-Capacity Silicon Electrodes

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.