Element Screening Engineering for High‐Entropy Alloy Anodes: Achieving Fast and Robust Li‐Storage With Optimal Working Potential

Abstract

While the high‐entropy strategy is highly effective in enhancing the performance of materials across various fields, an optimal methodology for selecting component elements for performance optimization is still lacking. Here the findings on uncovering the element selection rules for rational design of high‐entropy alloy anodes with exceptional lithium storage performance are reported. It is investigated high‐entropy element screening rules by modifying stable diamond‐structured Ge with P to induce a tetrahedrally coordinated sphalerite structure for enhanced metallic conductivity, further stabilized by incorporating Zn and other elements. Moreover, both theoretical and experimental results confirm that Li‐storage performance improves with increasing atomic number: BZnGeP3 < AlZnGeP3 < GaZnGeP3 < InZnGeP3. InZnGeP3‐based electrodes demonstrate the highest Li‐ion affinity, fastest electronic and Li‐ion transport, largest Li‐storage capacity and reversibility, and best mechanical integrity. Further element screening based on the above criteria leads to high entropy alloy anodes with metallic conductivity like GaCuSnInZnGeP6, GaCu(or Sn)InZnGeP5, CuSnInZnGeP5, InZnGePSeS(or Te), InZnGeP2S(or Se) which show superior Li‐storage performances. The excellent phase stability is attributed to their high configurational entropy. This study offers profound insights into element screening for high‐entropy alloy‐based anodes in Li‐ion batteries, providing guidance and reference for the element combination and screening of other high‐entropy functional materials.