Wide-Temperature Operation of Lithium-Sulfur Batteries Enabled by Multi-Branched Vanadium Nitride Electrocatalyst

Lianbo Ma; Yanrong Wang; Ziwei Wang; Junling Wang; Yuwen Cheng; Junxiong Wu; Bo Peng; Jie Xu; Wei Zhang; Zhong Jin

doi:10.1021/acsnano.3c01469

Wide-Temperature Operation of Lithium-Sulfur Batteries Enabled by Multi-Branched Vanadium Nitride Electrocatalyst

ACS Nano. 2023 Jun 27;17(12):11527-11536. doi: 10.1021/acsnano.3c01469. Epub 2023 Jun 8.

Authors

Lianbo Ma^{1

2}, Yanrong Wang^{2

3}, Ziwei Wang¹, Junling Wang⁴, Yuwen Cheng¹, Junxiong Wu⁵, Bo Peng¹, Jie Xu¹, Wei Zhang⁴, Zhong Jin²

Affiliations

¹ Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials, School of Materials Science and Engineering, Anhui University of Technology, Maanshan 243002, People's Republic of China.
² State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu 210023, People's Republic of China.
³ School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, Jiangsu 225002, People's Republic of China.
⁴ School of Materials and Energy, Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage Devices, Guangdong University of Technology, Guangzhou 510006, People's Republic of China.
⁵ College of Environmental and Resource Sciences and College of Carbon Neutral Modern Industry, Fujian Normal University, Fuzhou 350000, Fujian, People's Republic of China.

PMID: 37288710
DOI: 10.1021/acsnano.3c01469

Abstract

High-performance lithium-sulfur (Li-S) batteries that can work normally under harsh conditions have attracted tremendous attention; however, the sluggish reaction kinetics of polysulfide conversions at low temperatures as well as the notorious polysulfide shuttling at high temperatures remain to be resolved. Herein, a multibranched vanadium nitride (MB-VN) electrocatalyst has been designed and deployed for Li-S batteries. Both experimental (time-of-flight secondary ion mass spectroscopy and adsorption tests) and theoretical results verify the strong chemical adsorption capability and high electrocatalytic activity of MB-VN with respect to polysulfides. Moreover, in situ Raman characterization manifests the effective inhibition of polysulfide shuttling by the MB-VN electrocatalyst. Using MB-VN-modified separators, the Li-S batteries deliver an excellent rate capability (707 mAh g^-1 at 3.0 C) and great cyclic stability (678 mAh g^-1 after 400 cycles at 1.0 C) at room temperature. With 6.0 mg cm^-2 of sulfur and a lean electrolyte volume of ∼6 μL mg_s^-1, Li-S batteries exhibit a high areal capacity of 5.47 mAh cm^-2. Even over a wide temperature range (-20 to +60 °C), the Li-S batteries still maintain stable cyclic performance at high current rates. This work demonstrates that metal nitride based electrocatalysts can realize low-/high-temperature-tolerant Li-S batteries.

Keywords: harsh working conditions, electrocatalyst; lithium−sulfur batteries; polysulfide shuttling; vanadium nitride.