Single‐Atom Gold Isolated Onto Nanoporous MoSe2 for Boosting Electrochemical Nitrogen Reduction

• Published in: Small (Weinheim an der Bergstrasse, Germany) Vol. 18; no. 4; pp. e2104043 - n/a
• Main Authors: Chen, Dechao, Luo, Min, Ning, Shoucong, Lan, Jiao, Peng, Wei, Lu, Ying‐Rui, Chan, Ting‐Shan, Tan, Yongwen
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 01.01.2022
• Subjects: Ammonia; Catalysis; Chemical reduction; Electrocatalysts; electrocatalytic nitrogen reduction; Molybdenum compounds; MoSe 2; nanoporous catalysts; Nanotechnology; Selectivity; single‐atoms
• ISSN: 1613-6810; 1613-6829
• DOI: 10.1002/smll.202104043

The electrocatalytic nitrogen reduction reaction (NRR) provides a promising strategy to convert the abundant but inert N2 into NH3 using renewable energy. Herein, single‐atom Au isolated onto bicontinous nanoporous MoSe2 (np‐MoSe2) is designed as an electrocatalyst for achieving highly efficient NRR catalysis, which exhibits a high Faradaic efficiency (FE) of 37.82% and an NH3 production rate of 30.83 µg h−1 mg−1 at –0.3 V versus a reversible hydrogen electrode (RHE) in 0.1 m Na2SO4 under ambient conditions. Experimental and theoretical investigations reveal that the introduction of single Au atoms onto np‐MoSe2 optimizes the adsorption of NRR intermediates while suppressing the competing HER, thus providing an energetic‐favorable process for enhancing the catalytic selectivity toward electrochemical N2 reduction into NH3. Single Au atoms/clusters isolated onto nanoporous MoSe2 catalyst is constructed by the combination of chemical vapor deposition (CVD) process and chemical etching. The resulting catalyst is highly active and stable toward electrochemical nitrogen reduction with a much higher ammonia yield (30.83 µg h−1 mg−1) and Faradaic efficiency (FE, 37.82%) than well‐studied Mo‐based catalysts. This work not only paves a favorable avenue for exploring and designing single‐atoms anchored onto 2D materials, but also provides insights into regulating the reaction pathway for the nitrogen reduction reaction (NRR).