Citation: Jiajun Wang, Mengyao Shi, Guolin Yi, Lu Wang, Shulai Lei, Ke Xu, Shujuan Li, Jianshuai Mu. Computational prediction of Mo₂@g-C₆N₆ monolayer as an efficient electrocatalyst for N₂ reduction[J]. Chinese Chemical Letters, ;2022, 33(10): 4623-4627. doi: 10.1016/j.cclet.2021.12.040 shu

Computational prediction of Mo₂@g-C₆N₆ monolayer as an efficient electrocatalyst for N₂ reduction

Jiajun Wang ^a ,
Mengyao Shi ^a ,
Guolin Yi ^a ,
Lu Wang ^a ,
Shulai Lei ^{b, *,} ,
Ke Xu ^b ,
Shujuan Li ^{b, c} ,
Jianshuai Mu ^{a, *,}

a.
Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry, Tianjin Normal University, Tianjin 300387, China
b.
Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices, Hubei University of Arts and Science, Xiangyang 441053, China
c.
Institute of Mathematics, Free University of Berlin, Berlin D-14195, Germany

sllei@hbuas.edu.cn

hxxymujianshuai@tjnu.edu.cn

Received Date: 29 October 2021
Revised Date: 13 December 2021
Accepted Date: 15 December 2021
Available Online: 20 December 2021

Figures(5)

Electrocatalytic nitrogen reduction reaction (NRR) is an environmentally friendly method for sustainable ammonia synthesis under ambient conditions. Searching for efficient NRR electrocatalysts with high activity and selectivity is currently urgent but remains great challenge. Herein, we systematically investigate the NRR catalytic activities of single and double transition metal atoms (TM = Fe, Co, Ni and Mo) anchored on g-C₆N₆ monolayers by performing first-principles calculation. Based on the stability, activity, and selectivity analysis, Mo₂@g-C₆N₆ monolayer is screened out as the most promising candidate for NRR. Further exploration of the reaction mechanism demonstrates that the Mo dimer anchored on g-C₆N₆ can sufficiently activate and efficiently reduce the inert nitrogen molecule to ammonia through a preferred distal pathway with a particularly low limiting potential of -0.06 V. In addition, we find that Mo₂@g-C₆N₆ has excellent NRR selectivity over the competing hydrogen evolution reaction, with the Faradaic efficiency being 100%. Our work not only predicts a kind of ideal NRR electrocatalyst but also encouraging more experimental and theoretical efforts to develop novel double-atom catalysts (DACs) for NRR.
- g-C₆N₆ monolayer,
- Double-atom catalysts,
- Nitrogen reduction reaction,
- Hydrogen evolution reaction,
- Limiting potential,
- Density functional theory
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Computational prediction of Mo₂@g-C₆N₆ monolayer as an efficient electrocatalyst for N₂ reduction