Expediting Sulfur Reduction/Evolution Reactions with Integrated Electrocatalytic Network: A Comprehensive Kinetic Map.

Abstract

Electrocatalysts are considered the most promising candidates in ameliorating the slow kinetics of Li-S batteries (LSBs), however, the issue of insufficient catalytic capability remains to be addressed. Herein, we report an integrated catalytic network comprising graphitic carbon-encapsulated/bridged ultrafine NiCoP embedded in N, P-codoped carbon (GC-uNiCoP@NPC) as a highly competent catalyst for sulfur-based species conversions. By profiling the evolution map of Li-S chemistry via operando kinetic analyses, GC-uNiCoP@NPC is demonstrated to possess versatile yet efficient catalytic activity for sulfur reduction/evolution reactions, especially the rate-determining heterogeneous phase transitions. As a result, GC-uNiCoP@NPC enables high capacity and stable cycling of sulfur cathode under high areal loading and lean electrolyte. Moreover, pouch cells assembled under practical conditions present promising performance with a specific energy of 302 Wh kg-1. This work not only conceptually expands the catalyst design for LSBs but also provides a comprehensive insight into the catalyst performance for Li-S chemistry.