Synergistic Adsorption-Catalysis by Co/Ce Dual Single Atoms Trapped in Hollow Carbon Spheres Boosts Li-S Battery Performance.

Hou, Tianxin; Duan, Naiyuan; Bi, Chenyang; Tu, Jinwei; Luo, Mingmin; Qu, Yafei; Yang, Yang; Wang, Dongdong et al. · ACS Nano · 2025

basic_science · Level V

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Abstract

Lithium-sulfur (Li-S) batteries have a deteriorating capacity under the circumstances of the lithium polysulfide (LiPS) shuttle effect, which disrupts S<sub>8</sub>-to-Li<sub>2</sub>S conversion kinetics and shortens the cycle life. In this study, we engineered Co/Ce dual single atom catalysts anchored on nitrogen-doped hollow carbon spheres to mitigate the shuttle effect by adsorption-catalysis design. Ce sites exhibit stronger adsorption affinity for long-chain LiPS via the low formation enthalpy of Ce-S bonding, effectively confining soluble intermediates within the cathode, whereas Co sites dominantly catalyze the redox kinetics of solid Li<sub>2</sub>S nucleation and dissolution, reducing the energy barriers for Li<sub>2</sub>S deposition. The Co/Ce dual-site sulfur cathode achieved 92.8% capacity retention after 1000 cycles at 0.5 C, excellent rate capability (552 mAh g<sub>S</sub><sup>-1</sup> at 10 C), and an undersized capacity decay rate (0.06% per cycle) for 1000 cycles at 2 C. A coin cell with high sulfur loading delivered a high areal capacity of 3.99 mAh cm<sup>-2</sup> and maintained 3.61 mAh cm<sup>-2</sup> after 600 cycles at 0.2 C, highlighting the ability of Co/Ce dual single atoms in boosting Li-S battery performance.