Single, double, and triple transition metal atoms embedded in defective V3C2O2 for nitrogen reduction reaction: A DFT study

被引:27
作者
Wan, Jin [1 ]
Wang, Yanwei [1 ]
Tian, Wu [1 ]
Zhang, Huijuan [1 ]
Wang, Yu [1 ,2 ]
机构
[1] Chongqing Univ, Sch Chem & Chem Engn, State Key Lab Power Transmiss Equipment & Syst Se, 174 Shazheng St,Shapingba Dist, Chongqing 400044, Peoples R China
[2] Chongqing Univ, Sch Elect Engn, 174 Shazheng St,Shapingba Dist, Chongqing 400044, Peoples R China
基金
中国国家自然科学基金;
关键词
Nitrogen reduction reaction; Density functional theory; Single; double; and triple-atom catalysts; TOTAL-ENERGY CALCULATIONS; CATALYSIS; AMMONIA; PERFORMANCE; GRAPHDIYNE; CONVERSION; FIXATION; PROGRESS; N-2; CO;
D O I
10.1016/j.apsusc.2021.151020
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
Although numerous theoretical studies on single-atom catalysts (SACs) for an efficient electrochemical nitrogen reduction reaction (NRR) have been implemented to compare their catalytic performance. However, a rigid screening criterion excludes plenty of SACs with moderate catalytic activity. To overcome this limitation, we electronically modify the d-band structure of MXenes-based SACs to achieve higher catalytic performance. Here, multiple-transition metal atoms (TMn, TM = Cr, Mo, W, n = 1-3) embedded in defective V3C2O2 are system-atically investigated. First-principles calculations reveal that with the addition of foreign Mo and W atoms, the d -band centers of TMn@V3C2O2 are negatively shifted, and more electron-deficient sites are created. Consequently, Mo2@V3C2O2, Mo3@V3C2O2, W2@V3C2O2, and W3@V3C2O2 effectively inhibit the competitive hydrogen evo-lution reaction with favorable limiting potentials of-0.31,-0.33,-0.34, and-0.31 V, respectively. Our findings provide a new avenue of efficient atomic catalysts toward NH3 production while offering a reliable strategy for tuning the NRR performance of the MXenes-based SACs.
引用
收藏
页数:9
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