RuO<sub>x</sub> Quantum Dots Loaded on Graphdiyne for High-Performance Lithium-Sulfur Batteries.

Wang, Zhongqiang; Song, Congying; Shen, Han; Ma, Shaobo; Li, Guoxing; Li, Yuliang · Adv Mater · 2024

basic_science · Level V

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Abstract

Here, a strategy to strengthen d-p orbital hybridization by fabricating π backbonding in the catalyst for efficient lithium polysulfides (LiPSs) conversion is reported. A special interface structure of RuO<sub>x</sub> quantum dots (QDs) anchored on graphdiyne (GDY) nanoboxes (RuO<sub>x</sub> QDs/GDY) is prepared to enable strong Ru-to-alkyne π backdonation, which effectively regulates the d-electron structures of Ru centers to promote the d-p orbital hybridization between the catalyst and LiPSs and significantly boosts the catalytic performance of RuO<sub>x</sub> QDs/GDY. The strong affinity with Li ions and fast Li-ion diffusion of RuO<sub>x</sub> QDs/GDY also enable ultrastable Li metal anodes. Thus, S@RuO<sub>x</sub> QDs/GDY cathodes exhibit excellent cycling performance under harsh conditions, and Li@RuO<sub>x</sub> QDs/GDY anodes show an ultralong cycling life over 8800 h without Li dendrite growth. Lithium-sulfur (Li-S) full cells with S@RuO<sub>x</sub> QDs/GDY cathodes and Li@RuO<sub>x</sub> QDs/GDY anodes can deliver an impressive areal capacity of 17.8 mA h cm<sup>-2</sup> and good cycling stability under the practical conditions of low negative-to-positive electrode capacity (N/P) ratio (N/P = 1.4), lean electrolyte (E/S = 3 µL mg<sup>-1</sup> ), and high S mass loading (15.4 mg cm<sup>-2</sup> ).