Journal
CHINESE CHEMICAL LETTERS
Volume 33, Issue 10, Pages 4623-4627Publisher
ELSEVIER SCIENCE INC
DOI: 10.1016/j.cclet.2021.12.040
Keywords
g-C6N6 monolayer; Double-atom catalysts; Nitrogen reduction reaction; Hydrogen evolution reaction; Limiting potential; Density functional theory
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Funding
- Science & Technology Development Fund of Tianjin Education Commission for Higher Education [2020KJ008]
- Natural Science Foundation of Tianjin [18JCQNJC76000]
- College Students' Innovation and Entrepreneurship Training Program of Tianjin [202110065112]
- Science and Technology Research Project of Hubei Provincial Department of Education [D20212603]
- Hubei University of Arts and Science [2020kypytd002, XK2021024]
- China Scholarship Council
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This study systematically investigates the catalytic activities of single and double transition metal atoms anchored on g-C6N6 monolayers for NRR. Mo-2@g-C6N6 is identified as the most promising candidate for NRR due to its stability, activity, and selectivity. Further exploration of the reaction mechanism reveals that the Mo dimer anchored on g-C6N6 can efficiently reduce the inert nitrogen molecule to ammonia.
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, Mo-2@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 -0.06V. In addition, we find that Mo-2@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. (C) 2022 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
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