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Published on: December 6, 2021
Synergistic Adsorption-Catalysis by Co/Ce Dual Single Atoms Trapped in Hollow Carbon Spheres Boosts Li-S Battery
Tianxin Hou1, Naiyuan Duan1, Chenyang Bi1
1Hefei National Laboratory for Physical Science at Microscale and Department of Materials Science & Engineering, University of Science and Technology of China, Hefei 230026, China.
Abstract:
Lithium-sulfur (Li-S) batteries have a deteriorating capacity under the circumstances of the lithium polysulfide (LiPS) shuttle effect, which disrupts S8-to-Li2S 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 Li2S nucleation and dissolution, reducing the energy barriers for Li2S 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 gS-1 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-2 and maintained 3.61 mAh cm-2 after 600 cycles at 0.2 C, highlighting the ability of Co/Ce dual single atoms in boosting Li-S battery performance.

