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Cobalt-decorated carbon nanotube bottlebrushes for boosting polysulfide conversion in lithium-sulfur batteries

钴修饰碳纳米管瓶刷助力锂硫电池多硫化物转化

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Abstract

Developing superhierarchical carbon materials with multiple levels of structural hierarchy including porous structure, hybrid skeleton and/or topological morphology, is highly desirable to fulfill the demands of complex catalytic reactions in electrochemical energy storage and conversion systems. Herein, a class of hierarchical porous cobalt-decorated carbon nanotube bottlebrushes (Co/CNTBs) have been developed by controllably grafting hairy CNTs from the surface of a hybrid CNT backbone with Co nanoparticles as catalytic sites. The well-defined bottlebrush-like topology with hierarchically porous structure provides efficiently accessible surfaces/interfaces and highly conductive networks, while the Co-decorated hybrid skeleton promotes the reaction kinetics of sulfur redox conversion. As a result, an excellent rate capability of 707 mA h g−1 at 10 C and long-term cycling stability can be achieved for lithium-sulfur (Li-S) cells with Co/CNTBs-functionalized separators. Remarkably, the Li-S cell with Co/CNTBs-functionalized separator can deliver a high areal capacity of 4.81 mA h cm−2 after 100 cycles at 0.1 C with a sulfur loading of 6.72 mg cm−2. These findings may shed light on the facile in situ grafting strategy for the fabrication of high-performance superhierarchical carbon hybrids towards numerous challenging applications.

摘要

开发具有多层次结构(包括多孔结构、杂化骨架和/或拓扑形貌)的超结构碳材料, 对于满足电化学储能和转换系统中复杂催化反应的需求非常关键. 在本文中, 我们以钴纳米颗粒为催化位点, 在杂化碳纳米管骨架表面可控接枝毛发状碳纳米管, 开发了一类层次化多孔的钴修饰碳纳米管瓶刷(Co/CNTBs). 其中, 精确的瓶刷状拓扑形貌和分级多孔结构能够有效地提供可及表/界面和高导电网络, 钴修饰的杂化骨架可以促进硫的氧化还原反应动力学. 因此, 基于Co/CNTBs功能化隔膜的锂硫电池具有优异的倍率性能(在10 C下比容量为707 mA h g−1)和长效的循环稳定性. 更重要的是, 基于Co/CNTBs催化剂的高硫载量电池(6.72 mg cm−2)在0.1 C下循环100圈后仍具有4.81 mA h cm−2的高面积容量. 本工作为高性能超结构杂化碳材料的原位接枝合成策略带来了新的思路, 有望用于众多具有挑战性的应用.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (51872336, 51925308, and 52172061), the National Key Research and Development Program of China (2021YFF0500600), the Pearl River Talent Plan of Guangdong (2017GC010612), the Natural Science Foundation of Guangdong (2021A1515011617), the Fundamental Research Funds for the Central Universities (20lgzd18), and the Science and Technology Program of Guangzhou (202102021111 and 202002020041).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Key Laboratory for Polymeric Composite & Functional Materials of Ministry of Education, School of Chemistry, Sun Yat-sen University, Guangzhou, 510006, China

    Junlong Huang  (黄俊龙), Kunyi Leng  (冷坤怡), Zongheng Cen  (岑宗恒), Ruliang Liu  (刘如亮), Youlong Zhu  (朱有龙), Shaohong Liu  (刘绍鸿), Ruowen Fu  (符若文) & Dingcai Wu  (吴丁财)

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  1. Junlong Huang  (黄俊龙)
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Contributions

Wu D conceived the concept and supervised the research. Liu S and Wu D designed the project. Huang J and Leng K synthesized the materials. Huang J, Leng K, and Cen Z performed the material characterization and electrochemical tests. Huang J, Liu S and Wu D wrote the manuscript. Liu R, Zhu Y and Fu R gave some advice on the research. All authors discussed the results and commented on the manuscript.

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Correspondence to Shaohong Liu  (刘绍鸿) or Dingcai Wu  (吴丁财).

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The authors declare that they have no conflict of interest.

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Experimental details and supporting data are available in the online version of the paper.

Junlong Huang received his PhD degree from Sun Yat-sen University in 2020, under the supervision of Prof. Ruowen Fu. Now he is a postdoctoral fellow in Prof. Dingcai Wu’s group at Sun Yat-sen University. His current research interests lie in the design and preparation of functional polymer materials and their derived carbon materials toward energy storage and conversion.

Kunyi Leng received her Master degree from Sun Yat-sen University in 2020, under the supervision of Prof. Dingcai Wu. She is currently pursuing her PhD degree at the University of Tokyo under the supervision of Prof. Takuzo Aida. Her current research interests include the design and controllable preparation of porous materials.

Shaohong Liu received his PhD degree from Dalian University of Technology in 2016 under the supervision of Prof. Jieshan Qiu. He joined Prof. Dingcai Wu’s group at Sun Yat-sen University as an associate researcher in 2016 and became an associate professor in 2019. His current research interests focus on the design of advanced polymeric and carbonaceous materials for energy storage and conversion.

Dingcai Wu obtained his PhD degree in polymer chemistry and physics from Sun Yat-sen University in 2006. He joined the faculty of Sun Yat-sen University in 2006 and became a full professor in 2014. His current research interests focus on the preparation and applications of advanced functional materials. He currently serves as the deputy director of the Materials Science Institute and Key Laboratory for Polymeric Composite & Functional Materials of Ministry of Education, Sun Yat-sen University.

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Huang, J., Leng, K., Cen, Z. et al. Cobalt-decorated carbon nanotube bottlebrushes for boosting polysulfide conversion in lithium-sulfur batteries. Sci. China Mater. 66, 1747–1756 (2023). https://doi.org/10.1007/s40843-022-2303-0

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