Interface engineering via high-entropy sulfides for synergistic modulation of lithium nucleation and SEI stability toward ultra-stable lithium metal anodes

Abstract

Although lithium (Li) metal is regarded as the most promising anode material for high-energy-density batteries, issues such as unregulated dendrite growth and fragile solid electrolyte interphase (SEI) severely impede its practical application. Faced with the two fundamental interfacial electrochemical reactions—Li nucleation and SEI formation—which occur in parallel and are highly coupled, achieving dynamic synchronous coupling between them is an effective approach to solve the aforementioned problems. Herein, a high-entropy sulfide nanoneedle array was in-situ constructed on a carbon cloth (HES@CC), offering dual regulation functions: The multiple active sites of HES selectively adsorb Li⁺ ions, effectively reducing the nucleation barrier and guiding uniform Li nucleation, while HES assists in the in-situ formation of a high ionic conductivity SEI and its synchronous coupling with Li nucleation. Thus, HES@CC establishes a dynamic self-reinforcing stability loop: active-site-induced uniform Li nucleation–in-situ synchronous stable SEI formation–SEI-protected active sites. Consequently, HES@CC exhibits excellent stability during the Li deposition/stripping processes, including an average Coulombic efficiency as high as 99.73% over 1600 cycles, and a long cycling life of >2150 h.