Transition metal atoms embedded into B/N co-doped graphene as electrocatalysts toward nitrogen reduction reaction: Search for the optimal combination

被引:0
|
作者
Wang, Xiaolin [1 ]
Wang, Li [2 ]
Long, Debing [3 ]
Jin, Haoyue [1 ]
Sun, Zhuoyue [1 ]
Zhang, Shenghai [1 ]
She, Wei [1 ]
Wang, Jintao [1 ,4 ]
机构
[1] Ankang Univ, Shaanxi Prov Univ Key Lab Interfacial Porous Mat, Ankang Res Ctr New Nanomat Sci & Technol, Sch Chem & Environm,Southern Shaanxi Green Fine Ch, Ankang 725000, Peoples R China
[2] Henan Univ, Coll Chem & Mol Sci, Henan Key Lab Protect & Safety Energy Storage Ligh, Kaifeng 475004, Henan, Peoples R China
[3] Hubei Engn Univ, Sch Phys & Elect Informat Engn, Xiaogan 432000, Peoples R China
[4] Wuhan Inst Technol, Chongqing Res Inst, Chongqing 401220, Peoples R China
关键词
Electrocatalytic nitrogen reduction reaction; Transition metal atoms; B/N co-doped graphene; First-principles calculations; High-throughput screening; HABER-BOSCH; PLANE-WAVE; EFFICIENT ELECTROCATALYSTS; MOLECULAR-DYNAMICS; AMMONIA-SYNTHESIS; NO REDUCTION; SINGLE; MONOLAYERS; ELECTROREDUCTION; FIXATION;
D O I
10.1016/j.colsurfa.2024.135385
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
The catalytic performance of a series of single transition metal (TM = 3d, 4d, and 5d series) atoms anchored on B/N co-doped graphene (BxNy@Gra) toward electrocatalytic nitrogen reduction reaction (eNRR) was systematically investigated by first-principles calculations. Among 180 possible materials, four catalysts (Tc-B1N3@Gra, Os-B2N2 alpha@Gra, Re-B2N2 gamma@Gra, Nb-B3N1@Gra) feature the highest activity with U-L no higher than 0.31 V. Interestingly, a volcano curve between U-L and Delta E-ads(*NNH) can be established, so Delta E-ads(*NNH) can be applied as a descriptor to unveil the structure-activity relationship and characterize the activity of catalysts. The properties, thermal stability, and selectivity for the four catalysts were analyzed. Os-B2N2 alpha@Gra is identified as a promising catalyst in this work for catalyzing N-2 electroreduction to NH3 owing to its potent catalytic activity (U-L = -0.28 V), high stability and distinct selectivity. This work can give some meaningful guidance for rapid screening and the rational design of efficient single-atom catalysts for electrocatalytic ammonia synthesis and other related electrochemical reaction. We expect that the present study will inspire and promote the efforts from both experimental and theoretical in this direction.
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页数:12
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