期刊
ACS CATALYSIS
卷 9, 期 8, 页码 7052-7064出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b02179
关键词
electrocatalysis; water remediation; DFT modeling; microkinetic simulation; volcano curve
资金
- DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357]
- faculty start-up funds of Goldsmith and Singh from the University of Michigan, Ann Arbor
- Mcubed seed grant
Electrocatalytic reduction is a promising approach to remediate nitrate (NO3-), one of the world's most widespread water pollutants. In the present work, we elucidate activity and selectivity trends of transition metals for electrocatalytic nitrate reduction to benign or value-added products such as N-2 and NH3. Using density functional theory (DFT) calculations, we find that the adsorption strengths of oxygen and nitrogen atoms act as descriptors for the overall activity and selectivity of nitrate reduction electrocatalysts. Nitrate reduction rates, volcano plots, surface species coverages, and the degree of rate control were predicted for transition metal, electrocatalysts as a function of applied potential using DFT-based microkinetic modeling. Our microkinetic model rationalizes a number of experimental observations including the activity trends of pure metals and our in situ X-ray absorption spectroscopy measurements of competitive adsorption between hydrogen and nitrate on Pt/C. We also predict that Fe3Ru, Fe3Ni, Fe3Cu, and Pt3Ru are promising catalysts for nitrate electroreduction toward N-2 with relatively high activity and selectivity. Ultimately, this work gives insight into nitrate reduction on transition metal surfaces and can guide the design of improved electrocatalysts for nitrate remediation.
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