Revealing the effect of atom-level interlayer modification on accelerating interfacial catalytic redox reaction of...

Natural SnS₂ holds great promise as the oxygen electrode in lithium‑oxygen (LiO₂) batteries due to its low production cost and exposed catalytic active sites, however, its catalytic anisotropy associated with different facet structures restricts the energy conversion efficiency and interfacial electrochemical kinetics reactions of LiO₂ batteries. Herein, an atom-level interlayer modification strategy on regulating catalytic facet structure with inhibited nucleation process is proposed to activate the intrinsic catalytic activity of SnS₂ electrode in LiO₂ battery. Unlike conventional SnS₂ with anisotropic facet structures, Ru-introduced SnS₂ offer an enhanced interfacial superior (001) facet without inferior catalytic (102) facet, while more exposed catalytic sites with high O₂ selectivity can efficiently lower the Gibbs free energy change and accelerate the interfacial electrochemical kinetics. Moreover, the inhibition of nucleation can shorten the charge transfer path, enlarge the specific surface area, and induce more sulfur vacancies, resulting in strong O₂ adsorption ability with a lower energy barrier. Consequently, Ru-introduced SnS₂ electrodes exhibit higher discharge capacity, improved cyclic properties and stable rate capability. Our work may apply a new sight of constructing the catalytic facet on improving the catalytic activity of 2D catalysts in LiO₂ batteries.