期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 142, 期 12, 页码 5702-5708出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b13347
关键词
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资金
- Ontario Research Fund - Research Excellence Program
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- CIFAR Bio-Inspired Solar Energy program
- U.S. DOE [DE-AC02-06CH11357]
- Canadian Light Source
- Southern Ontario Smart Computing Innovation Platform (SOSCIP)
- Niagara supercomputer at the SciNet HPC Consortium
- Federal Economic Development Agency of Southern Ontario
- Province of Ontario
- IBM Canada Ltd.
- Ontario Centres of Excellence
- Mitacs
- Canada Foundation for Innovation
- Government of Ontario
- Ontario Research Fund - Research Excellence
- University of Toronto
- NSERC E.W.R. Steacie Memorial Fellowship
- Govt. of Canada
Electrochemical conversion of nitrate (NO3-) into ammonia (NH3) recycles nitrogen and offers a route to the production of NH3, which is more valuable than dinitrogen gas. However, today's development of NO3- electroreduction remains hindered by the lack of a mechanistic picture of how catalyst structure may be tuned to enhance catalytic activity. Here we demonstrate enhanced NO3- reduction reaction (NO3-RR) performance on Cu50Ni50 alloy catalysts, including a 0.12 V upshift in the half-wave potential and a 6-fold increase in activity compared to those obtained with pure Cu at 0 V vs reversible hydrogen electrode (RHE). Ni alloying enables tuning of the Cu d-band center and modulates the adsorption energies of intermediates such as *NO3-, *NO2, and *NH2. Using density functional theory calculations, we identify a NO3-RR-to-NH3 pathway and offer an adsorption energy-activity relationship for the CuNi alloy system. This correlation between catalyst electronic structure and NO3-RR activity offers a design platform for further development of NO3-RR catalysts.
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