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Fe‐cation Doping in NiSe 2 as an Effective Method of Electronic Structure Modulation towards High‐Performance Lithium‐Sulfur Batteries
Author(s) -
Shi Liwei,
Fang Hailiang,
Yang Xiaoxia,
Xue Jie,
Li Caifeng,
Hou Shifeng,
Hu Cheng
Publication year - 2021
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.202100216
Subject(s) - sulfur , cathode , redox , doping , lithium (medication) , nucleation , materials science , chemical engineering , transition metal , inorganic chemistry , chemistry , catalysis , metallurgy , organic chemistry , optoelectronics , medicine , engineering , endocrinology
The commercialization of Li−S batteries is hindered by the shuttling of lithium polysulfides (LiPSs), the sluggish sulfur redox kinetics as well as the low sulfur utilization during charge/discharge processes. Herein, a free‐standing cathode material was developed, based on Fe‐doped NiSe 2 nanosheets grown on activated carbon cloth substrates (Fe‐NiSe 2 /ACC) for high‐performance Li−S batteries. Fe‐doping in NiSe 2 plays a key role in the electronic structure modulation of NiSe 2 , enabling improved charge transfer with the adsorbed LiPSs molecules, stronger interactions with the active sulfur species and higher electrical conductivity. Effective promotion of the sulfur redox kinetics and enhanced sulfur utilization were achieved under high areal sulfur loadings. The stronger interactions with LiPSs together with the unique 3D structure of Fe‐NiSe 2 /ACC also induced the transformation of Li 2 S 2 /Li 2 S growth from conventional 2D films to 3D particles, significantly eliminating the barriers of solid nucleation and growth during the phase transition of liquid LiPSs to solid Li 2 S 2 /Li 2 S. With a high sulfur loading of 9.9 mg cm −2 , the Fe‐NiSe 2 /ACC cathode enabled a high area capacity of 9.14 mAh cm −2 with a low average decay of 0.11 % per cycle over 200 cycles at 0.1 C.