文献类型：期刊文献

英文题名：Regulating Fe Aggregation State via Unique Fe-N-V Pre-Coordination to Optimize the Adsorption-Catalysis Effect in High-Performance Lithium-Sulfur Batteries

作者：Yang, Lubin[1];Wang, Xiaowei[1];Cheng, Xiaomin[1];Zhang, Yongzheng[1];Ma, Cheng[1];Zhang, Yayun[1,2];Wang, Jitong[1];Qiao, Wenming[1];Ling, Licheng[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Specially Funct Mat & Related Technol, Minist Educ, Shanghai 200237, Peoples R China

年份：2023

卷号：33

期号：38

外文期刊名：ADVANCED FUNCTIONAL MATERIALS

收录：;EI(收录号：20232114137142);WOS:【SCI-EXPANDED(收录号:WOS:000991397200001)】；

基金：Acknowledgements This work was supported by the National Natural Science Foundation of China (nos. U21A2060, 22178116, 21978097), the Shanghai Pujiang Program (no. 21PJD019), the Natural Science Foundation of Shanghai (no. 22ZR1417400), the Fundamental Research Funds for the Central Universities (nos. 222201817001, 50321041918013, JKA01221601)

语种：英文

外文关键词：adsorption-catalysis effects; integrated electrocatalysts; lithium-sulfur batteries; single Fe atoms; VN nanocrystals

摘要：Lithium-sulfur batteries (LSBs) suffer from uncontrollable shuttling behavior of lithium polysulfides (LiPSs: Li2Sx, 4 <= x <= 8) and the sluggish reaction kinetics of bidirectional liquid-solid transformations, which are commonly coped through a comprehensive adsorption-catalysis strategy. Herein, a unique Fe-N-V pre-coordination is introduced to regulate the content of "dissociative Fe3+" in liquid phase, realizing the successful construction of N-doped micro-mesoporous "urchin-like" hollow carbon nanospheres decorated with single atom Fe-N-4 sites and VN nanoparticles (denoted as SA-Fe/VN@NMC). The strong chemisorption ability toward LiPSs and catalyzed Li2S decomposition behavior on VN, along with the boosted reaction kinetics for sulfur reduction on SA-Fe sites are experimentally and theoretically evidenced. Moreover, the nanoscale-neighborhood distribution of VN and SA-Fe active sites presents synergistic effect for the anchoring-reduction-decomposition process of sulfur species. Thus SA-Fe/VN@NMC presents an optimized adsorption-catalysis effect for the whole sulfur conversion. Therefore, the SA-Fe/VN@NMC based Li-S cells exhibit high cyclic stability (a low decay of 0.024% per cycle over 700 cycles at 1 C, sulfur content: 70 wt%) and considerable rate performance (683.2 mAh g(-1) at 4 C). Besides, a high areal capacity of 5.06 mAh cm(-2) is retained after 100 cycles under the high sulfur loading of 5.6 mg cm(-2). This work provides a new perspective to design the integrated electrocatalysts comprising hetero-formed bimetals in LSBs.