Element Screening of High-Entropy Silicon Anodes for Superior Li-Storage Performance of Li-Ion Batteries

• DOI: 10.1021/jacs.4c01711
• Publication Date: 2024-07-26T13:23:25Z
• Authors: Wenwu Li; Jeng-Han Wang; Yanhong Li; Howard Hsueh; Xiao Liu; Yafei Zhao; Shengchi Huang; Xinwei Li; Hui-Ming Cheng; Xiangfeng Duan; Ho Seok Park

The high-entropy silicon anodes are attractive for enhancing electronic and Li-ionic conductivity while mitigating volume effects advanced Li-ion batteries (LIBs), but plagued by the complicated elements screening process. Inspired resemblances in structure between sphalerite diamond, we have selected sphalerite-structured SiP with metallic as parent phase exploring element of silicon-based anodes. inclusion Zn is crucial improving structural stability Li-storage capacity. Within same group, performance significantly improved increasing atomic number order BZnSiP3 < AlZnSiP3 GaZnSiP3 InZnSiP3. Thus, InZnSiP3-based electrodes achieved a high capacity 719 mA h g–1 even after 1,500 cycles at 2,000 g–1, high-rate 725 10,000 owing to its superior lithium-ion affinity, faster conduction diffusion, higher reversibility, mechanical integrity than others. Additionally, incorporation larger sizes leads greater lattice distortion more defects, further facilitating mass charge transport. Following these rules, disordered-cation compounds such GaCuSnInZnSiP6, GaCu(or Sn)InZnSiP5, CuSnInZnSiP5, well mixed-cation -anion compositions, InZnSiPSeTe InZnSiP2Se(or Te), synthesized, demonstrating conductivity. formation mechanism attributed negative energies arising from elevated entropy.