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Improving the electrophilicity of nitrogen on nitrogen-doped carbon triggers oxygen reduction by introducing covalent vanadium nitride

引入共价型氮化钒来提高氮掺杂碳的亲电性以促进 氧还原反应

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Abstract

Nitrogen-doped carbon (NC) demonstrates great promise as an alternative electrocatalyst for the oxygen reduction reaction (ORR). The C atoms next to the N dopant have been identified as the exact active sites, and optimizing the electronic structure of N has a great effect on the activity. In this study, a novel VN@NC nanocomposite consisting of a vanadium nitride (VN) nanoparticle core and chainmail-like NC shell has been constructed via a simple physical mixing and annealing process. Benefiting from the unique core@shell nanowire structure and modulated electronic structure, the as-prepared VN@NC manifests an obviously promoted ORR activity (onset potential: 0.93 V) compared with pure NC and bulk VN. Specifically, incorporating VN induces charge transfer from N on NC to V in VN and increases the electrophilicity of N on NC, resulting in optimized adsorption to O-containing intermediates. VN@NC also manifests decent long-term stability (89% current density retention after a 40,000-s test). This finding highlights the significance of regulating the electronic structure of N in NC and provides a reliable strategy for constructing NC-based hybrid electrocatalysts.

摘要

氮掺杂碳(NC)是一种有潜力的氧还原反应(ORR)电催化剂. 氮掺 杂碳可直接作为ORR活性位点中心, 优化氮原子的电子结构对催化活 性具有很大影响. 本文通过简单的物理混合和煅烧处理, 构建了一种由 氮化钒(VN)纳米颗粒为核、“铠甲状”NC作为壳的新型VN@NC纳米复 合材料. 得益于纳米线独特的核@壳结构和优化的电子结构, 与纯NC和 体相VN相比, 所制备的VN@NC展现出更优异的ORR活性(起始电位: 0.93 V). VN的引入诱导了电荷从NC上的氮原子转移到VN上的钒原子, 增加了NC上氮原子的亲电性, 从而优化了对含氧中间体的吸附过程. VN@NC也展现出了良好的循环稳定性(四万秒测试后, 电流密度保持 率为89%). 本研究揭示了调节NC中氮原子电子结构的重要性, 并为构 建NC基复合型电催化剂提供了有效方法.

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Acknowledgements

This work was financially supported by Shenzhen Fundamental Research Program (JCYJ20190809114409397) and the Fundamental Research Funds for the Central Universities (WUT: 2020III029 and 2020IVA100).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, China

    Shidong Li  (李士栋), Lixue Xia  (夏力学), Jiexin Zhu  (朱杰鑫), Ziang Liu  (刘子昂), Ruhan He  (贺汝涵), Wen Luo  (罗雯), Wenzhong Huang  (黄文忠), Changwei Shi  (石长玮) & Liang Zhou  (周亮)

  2. Department of Chemistry, Tsinghua University, Beijing, 100084, China

    Zechao Zhuang  (庄泽超)

  3. State Key Laboratory of Silicate Materials for Architectures, International School of Materials Science and Engineering, Wuhan University of Technology, Wuhan, 430070, China

    Yan Zhao  (赵焱)

  4. The Institute of Technological Sciences, Wuhan University, Wuhan, 430072, China

    Yan Zhao  (赵焱)

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  1. Shidong Li  (李士栋)
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Contributions

Zhou L, Zhao Y, Li S, and Zhuang Z conceived the study. Zhuang Z and Li S performed the electrochemical measurements. Xia L performed the first-principles calculations. Li S, Zhuang Z, Xia L, and Zhu J participated in the all-data analysis and wrote the manuscript together with Zhou L. Zhou L and Zhao Y provided insights into the experiments and supervised the research. Liu Z drew the mechanism diagram. He R, Luo W, Huang W, and Shi C modified the manuscript. All authors agreed on the final version of the manuscript.

Corresponding authors

Correspondence to Yan Zhao  (赵焱) or Liang Zhou  (周亮).

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The authors declare that they have no conflict of interest.

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Supporting data are available in the online version of the paper.

Shidong Li received his BS degree in materials science and engineering from Shandong University of Science and Technology in 2016. He is currently pursuing his PhD degree in materials science and engineering at Wuhan University of Technology (WUT). His current research focuses on carbon-based electrocatalysts and their applications in Zn-air batteries.

Zechao Zhuang received his master of engineering degree from Fujian Normal University in 2015 and his PhD degree from WUT in 2019. He is currently conducting postdoctoral research in Prof. Yadong Li’s group at Tsinghua University. His research interests mainly focus on electron structure-oriented design and synthesis of advanced electrocatalysts for water splitting, fuel cells, and carbon dioxide reduction.

Yan Zhao received his PhD degree from Sichuan University in 1999. He then received another PhD degree from the University of Minnesota System in 2005. He is currently a chair professor at WUT. His research interests include multiscale and multifield coupled simulation, computational material simulation, nanomaterials, new energy catalysis, and 3D printing.

Liang Zhou received his BS (2006) and PhD (2011) degrees from Fudan University (with Prof. Dongyuan Zhao and Prof. Chengzhong Yu). He then conducted postdoctoral research in Prof. Xiong Wen (David) Lou’s group at Nanyang Technological University and Prof. Cheng-zhong Yu’s group at The University of Queensland. He is currently a professor at WUT. His research interests focus on functional nanomaterials for energy storage and conversion applications.

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Improving the electrophilicity of nitrogen on nitrogen-doped carbon triggers oxygen reduction by introducing covalent vanadium nitride

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Li, S., Zhuang, Z., Xia, L. et al. Improving the electrophilicity of nitrogen on nitrogen-doped carbon triggers oxygen reduction by introducing covalent vanadium nitride. Sci. China Mater. 66, 160–168 (2023). https://doi.org/10.1007/s40843-022-2116-3

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