文献类型：期刊文献

英文题名：Vanadium as Auxiliary for Fe-V Dual-Atom Electrocatalyst in Lithium-Sulfur Batteries: "3D in 2D" Morphology Inducer and Coordination Structure Regulator

作者：Yang, Lubin[1];Pan, Yukun[1];Zhou, Zhiqiang[1];Zhang, Yongzheng[1];Xu, Jie[2];Ma, Cheng[1];Zhang, Yayun[1,3];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]Anhui Univ Technol, Sch Mat Sci & Engn, Maanshan 243002, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Specially Funct Mat & Related Technol, Minist Educ, Shanghai 200237, Peoples R China

年份：2023

卷号：17

期号：17

起止页码：17405

外文期刊名：ACS NANO

收录：;EI(收录号：20233714702762);WOS:【SCI-EXPANDED(收录号:WOS:001188449400001)】；

基金：This workis supported by the National Natural Science Foundationof China (No. U21A2060, No. 22178116, No. 21978097), Shanghai PujiangProgram (No. 21PJD019), Natural Science Foundation of Shanghai (No.22ZR1417400), and Fundamental Research Funds for the Central Universities(No. 222201817001, No. 50321041918013, No. JKA01221601).

语种：英文

外文关键词：dual-atom active sites; electrocatalysts; metal-N-Ccoordination; bidirectional catalysis; lithium-sulfurbattery

摘要：The undesirable shuttling behavior, the sluggish redox kinetics of liquid-solid transformation, and the large energy barrier for decomposition of Li2S have been the recognized problems impeding the practical application of lithium-sulfur batteries. Herein, inspired by the spectacular catalytic activity of the Fe/V center in bioenzyme for nitrogen/sulfur fixation, we design an integrated electrocatalyst comprising N-bridged Fe-V dual-atom active sites (Fe/V-N-7) dispersed on ingenious "3D in 2D" carbon nanosheets (denoted as DAC), in which vanadium induces the laminar structure and regulates the coordination configuration of active centers simultaneously, realizing the redistribution of the 3d-orbital electrons of Fe centers. The high coupling/conjunction between Fe/V 3d electrons and S 2p electrons shows strong affinity and enhanced reactivity of DAC-Li2Sn (1 <= n <= 8) systems. Thus, DAC presents strengthened chemisorption ability toward polysulfides and significantly boosts bidirectional sulfur redox reaction kinetics, which have been evidenced theoretically and experimentally. Besides, the well-designed "3D in 2D" morphology of DAC enables uniform sulfur distribution, facilitated electron transfer, and abundant active sites exposure. Therefore, the assembled Li-S cells present outstanding cycling stability (637.3 mAh g(-1) after 1000 cycles at 1 C) and high rate capability (711 mAh g(-1) at 4 C) under high sulfur content (70 wt %).