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Simultaneous acceleration of sulfur reduction and oxidation on bifunctional electrocatalytic electrodes for quasi-solid-state Zn–S batteries

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Science China Chemistry 2024年第5期67卷 1531-1538页

作者： Mingli Wang Hong Zhang Tianhang Ding Fangjun Wu Lin Fu Bin Song Pengfei Cao Ke Lu Institutes of Physical Science and Information Technology School of Materials Science and EngineeringKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei 230601China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001China School of Chemistry and Chemical Engineering Guizhou UniversityGuiyang 550025China Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123China State Key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China

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.,SO_(4)^(2-)) and accumulation of inactive ZnS. Accordingly, the Co O anchored on the N-doped carbon-supported sulfur cathode delivers a high Zn^(2+)storage capacity of 1,172 m Ahg^(-1)and outstanding cycling stability with a capacity retention of 71.6% after500 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 Whkg^(-1)sulfuris 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.

关键词： Zn–S battery bifunctional catalysts solid-state battery sulfur redox degradation mechanism

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