期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 317, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121711
关键词
Photoelectrochemistry; Nitrogen reduction reaction; Hollow microspheres; Ammonia; Heterostructures
资金
- Beijing Municipal Natural Science Foundation [JQ20003]
- National Natural Science Foundation of China [21771021, 21822501, 22061130206]
- Newton Advanced Fellowship award [NAF\R1\201285]
- Fok Ying-Tong Education Foundation [171008]
- Measurements Fund of Beijing Normal University
- State Key Laboratory of Heavy Oil Processing, People's Republic of China
In this study, low-cost Mo-doped WO3@CdS porous hollow microspheres were synthesized and demonstrated as efficient catalysts for reducing gaseous N-2 into ammonia. The Mo-doping and interconnected porous heterostructures provide sufficient catalytic sites for effective photoelectrocatalytic N-2 reduction.
Photo/electrochemical fixation of atmospheric nitrogen (N-2) into valuable chemicals is a favorable strategy to utilize the abundant natural resources for efficient catalysis. It is extremely desirable to discover immensely active, durable, and selective catalysts for effective photoelectrochemical N-2 fixation. Herein, low-cost, non-noble metal-based porous Mo-doped WO3@CdS hollow microspheres as hierarchical heterostructures were synthesized that can effectively catalyze and reduce the gaseous N-2 into ammonia (NH3). High Faradaic efficiency (36.72%) and fast average ammonia yield rate (38.99 mu g h(-1) mg(cat)(-1)) were observed at -0.3 V vs. RHE in the neutral solution at ambient conditions. Mo-doping and interconnected porous heterostructures synergistically deliver sufficient catalytic sites for effective photoelectrocatalytic N-2 reduction. Furthermore, density functional theory (DFT) calculations validate that the Mo-doping WO3 is advantageous to decrease the energy barrier for N-2 activation and protonation. Therefore, this work demonstrates the rational construction of transition metals-based hierarchical hollow photoelectrocatalysts towards efficient artificial N-2 fixation.
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