Bifunctional functionalized two-dimensional transition metal borides for fast reaction redox kinetics in lithium-sulfur batteries

doi:10.1016/j.cjche.2024.03.034

Chinese Journal of Chemical Engineering ›› 2024, Vol. 73 ›› Issue (9): 81-89.DOI: 10.1016/j.cjche.2024.03.034

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Bifunctional functionalized two-dimensional transition metal borides for fast reaction redox kinetics in lithium-sulfur batteries

Na Li¹, Ninggui Ma², Yulu Zhan³, Haishun Wu¹, Jun Fan^2,4, Jianfeng Jia¹

1. Key Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education, School of Chemistry and Materials Science, Shanxi Normal University, Taiyuan 030000, China;
2. Department of Materials Science& Engineering, City University of Hong Kong, Kowloon, Hong Kong, China;
3. Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
4. Center for Advance Nuclear Safety and Sustainable Development, City University of Hong Kong, Kowloon, Hong Kong, China

Received:2023-07-19 Revised:2024-03-18 Accepted:2024-03-18 Online:2024-06-09 Published:2024-11-21
Contact: Jun Fan,E-mail:junfan@cityu.edu.hk;Jianfeng Jia,E-mail:jiajf@dns.sxnu.edu.cn
Supported by:
We acknowledge funding supported by the Shanxi Province Science Foundation for Youth (202303021212150), 1331 Engineering of Shanxi Province, Research Grants Council of Hong Kong (CityU 11306517, 11305919, and 11308620), and National Natural Science Foundation of China-Research Grants Council of Hong Kong Joint Research Scheme N_CityU104/19.

Bifunctional functionalized two-dimensional transition metal borides for fast reaction redox kinetics in lithium-sulfur batteries

Na Li¹, Ninggui Ma², Yulu Zhan³, Haishun Wu¹, Jun Fan^2,4, Jianfeng Jia¹

1. Key Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education, School of Chemistry and Materials Science, Shanxi Normal University, Taiyuan 030000, China;
2. Department of Materials Science& Engineering, City University of Hong Kong, Kowloon, Hong Kong, China;
3. Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China;
4. Center for Advance Nuclear Safety and Sustainable Development, City University of Hong Kong, Kowloon, Hong Kong, China

通讯作者: Jun Fan,E-mail:junfan@cityu.edu.hk;Jianfeng Jia,E-mail:jiajf@dns.sxnu.edu.cn
基金资助:
We acknowledge funding supported by the Shanxi Province Science Foundation for Youth (202303021212150), 1331 Engineering of Shanxi Province, Research Grants Council of Hong Kong (CityU 11306517, 11305919, and 11308620), and National Natural Science Foundation of China-Research Grants Council of Hong Kong Joint Research Scheme N_CityU104/19.

Abstract

Abstract: Lithium-sulfur (Li-S) batteries are regarded as one of the most promising next-generation energy storage systems due to their high theoretical specific energy density and low cost. However, serious shuttle effect and sluggish lithium polysulfides (LiPSs) redox kinetics severely impede the practical application of Li-S batteries. Employing polar sulfur hosts is an effective strategy to alleviate the above problems. Herein, the potential of two-dimensional (2D) Ti₂B-based sulfur hosts for Li-S batteries was comprehensively explored using first-principles calculations. The results show that functional groups of Ti₂B can significantly modulate its structural properties, thus affecting its interaction with sulfur-containing species. Among S, Se, F, Cl, and Br elements, Ti₂B terminated with S and Se atoms possess stronger adsorption capability towards soluble Li₂S₈, Li₂S₆, and Li₂S₄, obviously stronger than organic electrolytes, which indicates that they can completely suppress the shuttle effect. Besides, Ti₂BS₂ and Ti₂BSe₂ can powerfully expedite the electrochemical conversion of LiPSs. Moreover, the decomposition energy barrier of Li₂S and diffusion energy barrier of single Li ion on them are also fairly low, manifesting their excellent catalytic performance towards the oxidation of Li₂S. Finally, Ti₂BS₂ and Ti₂BSe₂ always keep metallic conductivity during the whole charge/discharge process. Taking all this into account, Ti₂BS₂ and Ti₂BSe₂ are proposed as promising bifunctional sulfur hosts for Li-S batteries. Our results suggest that increasing the proportion of S and Se groups during the synthesis of Ti₂B monolayers is greatly helpful for obtaining high-performance Li-S batteries. Besides, our work not only reveals the huge potential of 2D transition metal borides in Li-S batteries, but also provides insightful guidance for the design and screening of new efficient sulfur cathodes.

Key words: Lithium-sulfur (Li-S) batteries, Shuttle effect, Catalysis, Adsorption, Computational chemistry

摘要： Lithium-sulfur (Li-S) batteries are regarded as one of the most promising next-generation energy storage systems due to their high theoretical specific energy density and low cost. However, serious shuttle effect and sluggish lithium polysulfides (LiPSs) redox kinetics severely impede the practical application of Li-S batteries. Employing polar sulfur hosts is an effective strategy to alleviate the above problems. Herein, the potential of two-dimensional (2D) Ti₂B-based sulfur hosts for Li-S batteries was comprehensively explored using first-principles calculations. The results show that functional groups of Ti₂B can significantly modulate its structural properties, thus affecting its interaction with sulfur-containing species. Among S, Se, F, Cl, and Br elements, Ti₂B terminated with S and Se atoms possess stronger adsorption capability towards soluble Li₂S₈, Li₂S₆, and Li₂S₄, obviously stronger than organic electrolytes, which indicates that they can completely suppress the shuttle effect. Besides, Ti₂BS₂ and Ti₂BSe₂ can powerfully expedite the electrochemical conversion of LiPSs. Moreover, the decomposition energy barrier of Li₂S and diffusion energy barrier of single Li ion on them are also fairly low, manifesting their excellent catalytic performance towards the oxidation of Li₂S. Finally, Ti₂BS₂ and Ti₂BSe₂ always keep metallic conductivity during the whole charge/discharge process. Taking all this into account, Ti₂BS₂ and Ti₂BSe₂ are proposed as promising bifunctional sulfur hosts for Li-S batteries. Our results suggest that increasing the proportion of S and Se groups during the synthesis of Ti₂B monolayers is greatly helpful for obtaining high-performance Li-S batteries. Besides, our work not only reveals the huge potential of 2D transition metal borides in Li-S batteries, but also provides insightful guidance for the design and screening of new efficient sulfur cathodes.

关键词: Lithium-sulfur (Li-S) batteries, Shuttle effect, Catalysis, Adsorption, Computational chemistry

Na Li, Ninggui Ma, Yulu Zhan, Haishun Wu, Jun Fan, Jianfeng Jia. Bifunctional functionalized two-dimensional transition metal borides for fast reaction redox kinetics in lithium-sulfur batteries[J]. Chinese Journal of Chemical Engineering, 2024, 73(9): 81-89.

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Bifunctional functionalized two-dimensional transition metal borides for fast reaction redox kinetics in lithium-sulfur batteries

Bifunctional functionalized two-dimensional transition metal borides for fast reaction redox kinetics in lithium-sulfur batteries

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