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Regulating the orbital hybridization to induce asymmetrical catalysis for efficient reversible sodium conversion storage

Authors: Zijia Qi; Kai Cui; Simi Sui; Yuxuan Wang; Haonan Xie; Guangxuan Wu; Yihao Cheng; Enzuo Liu; Fang He; Chunnian He; Tianshuai Wang; Biao Chen; Naiqin Zhao

DOI: 10.1007/s40843-025-3397-0Status: Verified Translated Edition
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Key Findings in This Report

• • PC-SAMn catalyst achieves a compositional reversible degree of 89.61% for MoS2 anodes, significantly surpassing conventional C-SACs and enabling near-complete recovery of MoS2 after charging, which directly translates to higher usable capacity and reduced active material loss in sodium-ion batteries. • • The capacity decay ratio is only 0.18% per 100 cycles over 2000 cycles, corresponding to a capacity retention of approximately 96.4% after 2000 cycles. This ultra-low degradation rate addresses the long-standing cycle-life limitation of conversion-type anodes, potentially reducing battery replacement costs in grid-scale energy storage. • • Asymmetrical dual active centers (Mn and P) weaken the Na–S bond strength through Mn–S d-p and P–Na s-p orbital hybridizations, lowering the Na2S decomposition barrier. This catalytic effect mitigates the shuttle problem and irreversible Na–S storage mechanism, enhancing Coulombic efficiency and safety. • • The designed catalyst enables reversible conversion between MoS2 and Mo/Na2S, preventing the segregation of Mo and Na2S and the formation of irreversible products (Mo and S). This maintains the high theoretical capacity of MoS2 (670 mAh/g) over extended cycling, offering a pathway for high-energy-density SIBs.