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

被引:23
作者
Li, Shidong [1 ]
Zhuang, Zechao [2 ]
Xia, Lixue [1 ]
Zhu, Jiexin [1 ]
Liu, Ziang [1 ]
He, Ruhan [1 ]
Luo, Wen [1 ]
Huang, Wenzhong [1 ]
Shi, Changwei [1 ]
Zhao, Yan [3 ,4 ]
Zhou, Liang [1 ]
机构
[1] Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China
[2] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[3] Wuhan Univ Technol, Int Sch Mat Sci & Engn, State Key Lab Silicate Mat Architectures, Wuhan 430070, Peoples R China
[4] Wuhan Univ, Inst Technol Sci, Wuhan 430072, Peoples R China
关键词
electrophilicity; nitrogen sites; chainmail carbon shell; vanadium nitride; oxygen reduction reaction; LITHIUM STORAGE; RATIONAL DESIGN; CATALYSTS; NANOTUBES; PERFORMANCE; EVOLUTION; ELECTROCATALYSTS; HYBRID; MODULATION; NANOSHEETS;
D O I
10.1007/s40843-022-2116-3
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
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.
引用
收藏
页码:160 / 168
页数:9
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