Regulating Fe Aggregation State via Unique FeNV Pre‐Coordination to Optimize the Adsorption‐Catalysis Effect in High‐Performance Lithium‐Sulfur Batteries

Author:

Yang Lubin1,Wang Xiaowei1,Cheng Xiaomin1,Zhang Yongzheng1,Ma Cheng1,Zhang Yayun12,Wang Jitong1ORCID,Qiao Wenming1,Ling Licheng1

Affiliation:

1. State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 P. R. China

2. Key Laboratory for Specially Functional Materials and Related Technology of the Ministry of Education East China University of Science and Technology Shanghai 200237 P. R. China

Abstract

AbstractLithium‐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‐N4 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.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Shanghai Municipality

Fundamental Research Funds for the Central Universities

Publisher

Wiley

Subject

Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials

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