Clustering Bimetallic M–N–C Catalyst: A Synergistic Approach to Advancing Sulfur Conversion Kinetics for High‐Performance Lithium‐Sulfur Batteries

Abstract Lithium–sulfur (Li–S) batteries stand out as a promising candidate for future energy storage, characterized by their notable energy density and affordability. However, the impediments raised by polysulfide shuttling and sluggish reaction kinetics pose substantial challenges to the widespread implementation of this technology. Herein, a unique Fe–Co bimetallic single‐atom‐cluster catalyst (FeCo‐SACC) for Li–S batteries are developed. The synergistic integration of single atoms and clusters guarantees not only a commendable specific catalytic activity but also a high metal loading of up to 25 wt%. Meanwhile, the intermetallic interactions regulate the electronic structure, enabling higher sulfur affinity and faster conversion kinetics. The unique 3D‐ordered mesoporous (3DOM) carbon architecture further affords conducive sulfur accommodation, efficient active site exposure, and facile ion/mass transfer. As a result, facile and stable sulfur electrochemistry is realized, contributing to excellent cyclability over 1000 cycles and rate capability up to 5 C. Decent cell performances can still be achievable under practical criteria, e.g., high sulfur loading of 15 mg cm⁻², lean electrolyte of 4.6 µL mg⁻¹, and 1.91‐Ah pouch configuration. This work establishes a novel paradigm for the development of advanced sulfur electrocatalysts and high‐performance Li–S batteries.