Data-Driven Atomic Interplay Modulation Enables Dual-Functional High-Entropy Alloy Mediator for Li–S Batteries

Abstract High-entropy alloys (HEAs) have emerged as appealing candidates to achieve performance regulation in Li–S batteries. Nevertheless, the design principles and working mechanisms of HEAs for dual electrodes remain elusive because of their structural disorder and chemical complexity. Herein, we propose a data-driven maneuver to enable rapid and precise screening of a customized HEA nanocatalyst (FeCoNiCuVMn, 6E-HEAs) via a performance-oriented theoretical criterion in the realm of Li–S electrochemistry. The delicate modulation of atomic interplay in 6E-HEAs simultaneously accelerates sulfur redox kinetics and stabilizes lithium metal deposition. Consequently, Li–S batteries sustain favorable cycling performance at 1.0 C over 1000 cycles while affording a capacity decay rate of merely 0.067% per cycle. The pouch cell harvests a specific capacity of 884.8 mAh g–1 at 0.5 C with steady cyclic operation. Our study elucidates crucial roles of effective compositional gain in boosting bidirectional Li–S electrocatalysis, offering atomic-level insights into HEA design for electrocatalytic reactions.