Abstract
Accelerating insoluble Li(2) S(2) -Li(2) S reduction catalysis to mitigate the shuttle effect has emerged as an innovative paradigm for high-efficient lithium-sulfur battery cathodes, such as single-atom catalysts by offering high-density active sites to realize in situ reaction with solid Li(2) S(2) . However, the profound origin of diverse single-atom species on solid-solid sulfur reduction catalysis and modulation principles remains ambiguous. Here we disclose the fundamental origin of Li(2) S(2) -Li(2) S reduction catalysis in ferromagnetic elements-based single-atom materials to be from their spin density and magnetic moments. The experimental and theoretical studies disclose that the Fe-N(4) -based cathodes exhibit the fastest deposition kinetics of Li(2) S (226 mAh g(-1) ) and the lowest thermodynamic energy barriers (0.56 eV). We believe that the accelerated Li(2) S(2) -Li(2) S reduction catalysis enabled via spin polarization of ferromagnetic atoms provides practical opportunities towards long-life batteries.