Fundamentally manipulating the electronic structure of polar bifunctional catalysts for lithium-sulfur batteries: Heterojunction design versus doping engineering

Xu, Huifang, Jiang, Qingbin, Shu, Zheng, Hui, Kwan San ORCID: https://orcid.org/0000-0001-7089-7587, Wang, Shuo, Zheng, Yunshan, Liu, Xiaolu, Xie, Huixian, Ip, Weng Fai (Andy), Zha, Chenyang, Cai, Yongqing and Hui, Kwun San (2024) Fundamentally manipulating the electronic structure of polar bifunctional catalysts for lithium-sulfur batteries: Heterojunction design versus doping engineering. Advanced Science. ISSN 2198-3844

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Abstract

Heterogeneous structures and doping strategies have been intensively used to manipulate the catalytic conversion of polysulfides to enhance reaction kinetics and suppress the shuttle effect in lithium-sulfur (Li-S) batteries. However, understanding how to select suitable strategies for engineering the electronic structure of polar catalysts is lacking. Here, a comparative investigation between heterogeneous structures and doping strategies is conducted to assess their impact on the modulation of the electronic structures and their effectiveness in catalyzing the conversion of polysulfides. These findings reveal that Co0.125Zn0.875Se, with metal-cation dopants, exhibits superior performance compared to CoSe2/ZnSe heterogeneous structures. The incorporation of low Co2+ dopants induces the subtle lattice strain in Co0.125Zn0.875Se, resulting in the increased exposure of active sites. As a result, Co0.125Zn0.875Se demonstrates enhanced electron accumulation on surface Se sites, improved charge carrier mobility, and optimized both p-band and d-band centers. The Li-S cells employing Co0.125Zn0.875Se catalyst demonstrate significantly improved capacity (1261.3 mAh g−1 at 0.5 C) and cycle stability (0.048% capacity delay rate within 1000 cycles at 2 C). This study provides valuable guidance for the modulation of the electronic structure of typical polar catalysts, serving as a design directive to tailor the catalytic activity of advanced Li-S catalysts.

Item Type:	Article
Additional Information:	Funding Information: This work was supported by the Science and Technology Development Fund, Macau SAR (File no. 0046/2019/AFJ, 0007/2021/AGJ, 0070/2023/AFJ, 0022/2023/RIB1, 0033/2023/ITP1, 0032/2021/ITP, and 006/2022/ALC), University of Macau (File no. MYRG2020‐00187‐IAPME and MYRG2022‐00223‐IAPME), the UEA funding, and the Science and Technology Program of Guangdong Province of China (Grant No. 2022A0505030028). The DFT calculations are performed at the High Performance Computing Cluster (HPCC) of Information and Communication Technology Office (ICTO) at the University of Macau.
Uncontrolled Keywords:	active sites,doping strategies,electronic structures,heterogeneous structures,polar catalysts,medicine (miscellaneous),chemical engineering(all),materials science(all),biochemistry, genetics and molecular biology (miscellaneous),engineering(all),physics and astronomy(all) ,/dk/atira/pure/subjectarea/asjc/2700/2701
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 11:31
Last Modified:	11 Apr 2024 09:30
URI:	https://ueaeprints.uea.ac.uk/id/eprint/94842
DOI:	10.1002/advs.202307995

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