Electrochemical mechanisms of the reduction of N2 to NH3 catalyzed by TM anchored on Nvs-g-C3N4/graphene van der Waals heterostructure: Insights from a first-principles study

被引:4
|
作者
Li, De-Qing [1 ]
Gao, Jin-Ai [2 ]
Hao, Ming-Tian [1 ]
Wujieti, Baerlike [1 ]
Li, Xiao-yu [1 ]
Chen, Bo-Zhen [1 ]
机构
[1] Univ Chinese Acad Sci, Sch Chem Sci, 19A Yuquan Rd, Beijing 100049, Peoples R China
[2] Univ Chinese Acad Sci, Hangzhou Inst Adv Study, Sch Mol Med, Hangzhou 310024, Peoples R China
来源
MOLECULAR CATALYSIS | 2023年 / 547卷
基金
中国国家自然科学基金;
关键词
Graphene; SACs; NRR; Heterostructure; HYDROGEN EVOLUTION; NITROGEN-FIXATION; SINGLE; AMMONIA; ATOM; CARBON; ELECTROREDUCTION; DINITROGEN; OXIDATION; HYBRID;
D O I
10.1016/j.mcat.2023.113353
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nitrogen fixation is one of the most critical issues in chemical science and technology. However, developing efficient and stable electro(photo)catalysts remains a comprehensive challenge. Here, we constructed 21 singleatom heterostructures consisting of g-C3N4 with nitrogen vacancies and graphene (TM@Nvs-g-C3N4/graphene, TM=Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Ag, Pd, Cd and Pt) and systematically investigated their stabilities and catalytic activities for the conversion from N2 to NH3. The calculations indicate that all heterostructures are thermodynamically stable. Among of them, 15 TM@Nvs-g-C3N4/graphene heterojunctions can activate N2, and effectively reduce N2 into NH3 by a distal or alternating mechanism. The Cr, Mo and Nb atoms anchored in Nvs-g-C3N4/graphene heterojunctions have higher activities and selectivities for nitrogen reduction reaction (NRR). In particular, Mo@Nvs-g-C3N4/graphene has the highest NRR performance. The Bader charge and PDOS analysis elucidate that the D-& pi;* feedback bonds formed by 4d orbitals of Mo atom and & pi;* orbitals of N2 plays a dominant role in the activation of N2. Altogether, the results obtained in this study could provide new avenues for the development of electrochemical catalyst for the reduction of N2 to NH3.
引用
收藏
页数:12
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