Interfacial “double-terminal binding sites” catalysts synergistically boosting the electrocatalytic Li2S redox for durable lithium-sulfur batteries

Xu, Huifang, Jiang, Qingbin, Hui, Kwan San ORCID: https://orcid.org/0000-0001-7089-7587, Wang, Shuo, Liu, Lingwen, Chen, Tianyu, Zheng, Yunshan, Ip, Weng Fai, Dinh, Duc Anh, Zha, Chenyang, Lin, Zhan and Hui, Kwun Nam (2024) Interfacial “double-terminal binding sites” catalysts synergistically boosting the electrocatalytic Li2S redox for durable lithium-sulfur batteries. ACS Nano, 18 (12). pp. 8839-8852. ISSN 1936-0851

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Abstract

Catalytic conversion of polysulfides emerges as a promising approach to improve the kinetics and mitigate polysulfide shuttling in lithium-sulfur (Li-S) batteries, especially under conditions of high sulfur loading and lean electrolyte. Herein, we present a separator architecture that incorporates double-terminal binding (DTB) sites within a nitrogen-doped carbon framework, consisting of polar Co0.85Se and Co clusters (Co/Co0.85Se@NC), to enhance the durability of Li-S batteries. The uniformly dispersed clusters of polar Co0.85Se and Co offer abundant active sites for lithium polysulfides (LiPSs), enabling efficient LiPS conversion while also serving as anchors through a combination of chemical interactions. Density functional theory calculations, along with in situ Raman and X-ray diffraction characterizations, reveal that the DTB effect strengthens the binding energy to polysulfides and lowers the energy barriers of polysulfide redox reactions. Li-S batteries utilizing the Co/Co0.85Se@NC-modified separator demonstrate exceptional cycling stability (0.042% per cycle over 1000 cycles at 2 C) and rate capability (849 mAh g-1 at 3 C), as well as deliver an impressive areal capacity of 10.0 mAh cm-2 even in challenging conditions with a high sulfur loading (10.7 mg cm-2) and lean electrolyte environments (5.8 μL mg-1). The DTB site strategy offers valuable insights into the development of high-performance Li-S batteries.

Item Type:	Article
Additional Information:	Funding Information: This work was supported by the Science and Technology Development Fund (FDCT) of Macao SAR (0033/2023/ITP1, 0022/2023/RIB1, 046/2019/AFJ, 0007/2021/AGJ, 006/2022/ALC, and 0070/2023/AFJ), the Macau Young Scholars Program (AM2020005), Guangdong Basic and Applied Basic Research Foundation (2022A1515110994 and 2022A0505030028), the Multi-Year Research Grants (MYRG2020-00187-IAPME and MYRG2022-00223-IAPME) from the Research Services and Knowledge Transfer Office at the University of Macau, UEA funding. and the High-Performance Computing Cluster (HPCC) of Information and Communication Technology Office (ICTO) at the University of Macau. Publisher Copyright: © 2024 The Authors. Published by American Chemical Society.
Uncontrolled Keywords:	binding energy,double-terminal binding sites,energy barriers,separator architecture,superb electrocatalysis,materials science(all),engineering(all),physics and astronomy(all) ,/dk/atira/pure/subjectarea/asjc/2500
Faculty \ School:	Faculty of Science > School of Engineering
Related URLs:	http://www.scopus.com/inward/record.url?...
Depositing User:	LivePure Connector
Date Deposited:	05 Apr 2024 10:32
Last Modified:	09 Apr 2024 15:30
URI:	https://ueaeprints.uea.ac.uk/id/eprint/94838
DOI:	10.1021/acsnano.3c11903

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