Potassium‐ion batteries (PIBs) have appealed increasing attention due to the inexpensive K‐element resources and satisfactory electrochemical properties. Presently, there are still challenges for developing desirable anode materials. Two‐dimensional metal sulfides exhibit high specific capacity as host for PIBs, yet the dissolution and agglomeration of unstable reaction intermediate KxSy (K2S, K2S5) inescapability induces large loss of active ingredients and poor reactions reversibility, leading to inferior lifespan. Herein, polar polysulfide VS4 is introduced into SnS nanosheets with constructing layered VS4/SnS heterostructure anchored in graphene scaffold (VS4/SnS@C). In this framework, VS4 with unsaturated bridging (S2)2– can act as the anchoring sites to stabilize intermediates KxSy with efficient entrapment effects. Moreover, the heterostructure can maintain layered SnS and regulate the distribution of KxSy with high conversion reversibility. The reaction reversibility and intermediate absorptivity are enhanced, as confirmed by in situ X‐ray diffraction analysis and theoretical calculations. Consequently, the VS4/SnS@C electrode exhibits ultra‐long lifespans, which achieves a capacity of 168.4 mAh g–1 at 1 A g–1 after 6000 cycles. This strategy of heterostructure design facilitates the understanding of K‐storage mechanisms and significantly enhances the reaction reversibility, providing a thought to address the challenges in metal sulfide anodes toward the development of high‐performance PIBs.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.