Understanding sulfur conversion chemistry is key to the development of sulfur-based high-energy-density batteries. However, unclear relationships between the electronic structure of the catalyst and its activity are the major problem. Here, we provide a direct correlation between the p electron gain of S in p-block metal sulfides and the apparent activation energies (Ea) for the sulfur reduction reaction (SRR), in particular, Li2Sn to Li2S conversion, which is the rate-determining step of the SRR. The maximum p charge occurs in bismuth sulfide and results in the lowest Ea and a high SRR rate in the cathode. Li–S batteries with the Bi2S3 catalyst work steadily at a high rate of 5.0C with a high-capacity retention of ~85% after 500 cycles. A high areal capacity of ~21.9 mAh cm−2 was obtained under a high sulfur loading of 17.6 mg cm−2 but a low electrolyte/sulfur ratio of 7.5 μl mg−1.
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This work was supported by the National Key R&D Program of China (2022YFA1503502 and 2021YFF0500600), National Natural Science Foundation of China (22025204, 51932005, 92034301, 52102283 and 52022041) and Innovation Program of the Shanghai Municipal Education Commission (2021-01-07-00-02-E00119).
The authors declare no competing interests.
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Hua, W., Shang, T., Li, H. et al. Optimizing the p charge of S in p-block metal sulfides for sulfur reduction electrocatalysis. Nat Catal 6, 174–184 (2023). https://doi.org/10.1038/s41929-023-00912-9