Toward Complete Transformation of Sodium Polysulfides by Regulating the Second‐Shell Coordinating Environment of Atomically Dispersed Fe

Room temperature sodium‐sulfur (RT Na‐S) batteries are highly competitive as potential energy storage devices. Nevertheless, their actually achieved reversible capacities are far below the theoretical value due to incomplete transformation of polysulfides. Herein, atomically dispersed Fe‐N/S active...

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Published in:Angewandte Chemie 2023-06, Vol.135 (26), p.n/a
Main Authors: Bai, Ruilin, Lin, Qiaosong, Li, Xinyu, Ling, Fangxin, Wang, Huijuan, Tan, Sha, Hu, Lingxiang, Ma, Mingze, Wu, Xiaojun, Shao, Yu, Rui, Xianhong, Hu, Enyuan, Yao, Yu, Yu, Yan
Format: Article
Language:English
Subjects:
Absorption spectroscopy
Catalysis
Chemistry
Coordinating Environment
Dispersion
ENERGY STORAGE
Fe Single Atom
Polysulfides
Potential energy
Room temperature
RT Na-S Batteries
Sodium
Sulfur
Synchrotron radiation
Synchrotrons
Transformation Kinetics
Transformations
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Summary:Room temperature sodium‐sulfur (RT Na‐S) batteries are highly competitive as potential energy storage devices. Nevertheless, their actually achieved reversible capacities are far below the theoretical value due to incomplete transformation of polysulfides. Herein, atomically dispersed Fe‐N/S active center by regulating the second‐shell coordinating environment of Fe single atom is proposed. The Fe−N4S2 coordination structure with enhanced local electronic concentration around the Fermi level is revealed via synchrotron radiation X‐ray absorption spectroscopy (XAS) and theoretical calculations, which can not only significantly promote the transformation kinetics of polysulfides, but induce uniform Na deposition for dendrite‐free Na anode. As a result, the obtained S cathode delivers a high initial reversible capacity of 1590 mAh g−1, nearly the theoretical value. This work opens up a new avenue to facilitate the complete transformation of polysulfides for RT Na‐S batteries. Atomically dispersed N, S‐coordinated Fe catalysts are anchored into porous carbon nanofibers as hosts for room‐temperature sodium‐sulfur batteries. The introduction of second‐shell S atoms modulates the electronic structure of Fe centers, thus enhancing the catalytic activity for promoting complete transformation of active S species, while realizing dendrite‐free Na deposition.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202218165