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

Xu, Huifang, Jiang, Qingbin, Hui, Kwan San, 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.
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 (former - to 2024)
Related URLs:	http://www.scopus.com/inward/record.url?...
Depositing User:	LivePure Connector
Date Deposited:	05 Apr 2024 10:32
Last Modified:	30 Jan 2025 02:38
URI:	https://ueaeprints.uea.ac.uk/id/eprint/94838
DOI:

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