Abstract
The incomplete sulfur reduction and high ZnS re-oxidation energy barrier along with severe side reactions during the battery cycling compromise the practical application of Zn–S electrochemistry. Herein, a bifunctional electrocatalytic sulfur matrix that simultaneously accelerates the sulfur reduction and ZnS oxidation is proposed to realize a highly-efficient Zn–S cell. It is revealed that the N-heteroatom hotspots are more favorable for facilitating the conversion of S to ZnS while the CoO nanocrystal substantially lowers the ZnS activation energy barrier thereby suppressing the formation of disproportionation species (e.g., \({\rm{S}}{{\rm{O}}_4}^{2 - }\)) and accumulation of inactive ZnS. Accordingly, the CoO anchored on the N-doped carbon-supported sulfur cathode delivers a high Zn2+ storage capacity of 1,172 mAh g−1 and outstanding cycling stability with a capacity retention of 71.6% after 500 cycles with a high average Coulombic efficiency of 97.8%. Simultaneously, the stable cycling of solid-state Zn–S pouch cells with an energy density of 585 \({\rm{Wh}}\,\,{\rm{k}}{{\rm{g}}^{ - 1}}_{{\rm{sulfur}}}\) is also demonstrated. Moreover, the postmortem analysis reveals that the degradation of Zn–S cells is mainly attributed to the limited reversibility of Zn anodes rather than the ZnS decomposition and/or accumulation. The approach to the bidirectional catalysis manipulated the sulfur redox provides a new perspective to realize the theoretical potentials of Zn–S cells.
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Acknowledgements
This work was financially supported by the Natural Scientific Foundation of China (22109001, 22208335), Postdoctoral Fellowship Program of CPSF (GZB20230950), and the Hefei National Laboratory for Physical Sciences at the Microscale (KF2020106). We also thank the support provided by the Collaborative Innovation Center of Suzhou Nano Science and Technology (NANO-CIC).
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Supplementary Information: Simultaneous Acceleration of Sulfur Reduction and Oxidation on Bifunctional Electrocatalytic Electrodes for Quasi-Solid-State Zn–S Batteries
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Wang, M., Zhang, H., Ding, T. et al. Simultaneous acceleration of sulfur reduction and oxidation on bifunctional electrocatalytic electrodes for quasi-solid-state Zn–S batteries. Sci. China Chem. 67, 1531–1538 (2024). https://doi.org/10.1007/s11426-023-1956-7
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DOI: https://doi.org/10.1007/s11426-023-1956-7