Back to Search
Start Over
Enhanced Nitrate-to-Ammonia Activity on Copper-Nickel Alloys via Tuning of Intermediate Adsorption
- Source :
- Journal of the American Chemical Society. 142(12)
- Publication Year :
- 2020
-
Abstract
- 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.
- Subjects :
- Inorganic chemistry
chemistry.chemical_element
General Chemistry
010402 general chemistry
Electrochemistry
01 natural sciences
Biochemistry
Copper
Redox
Catalysis
0104 chemical sciences
Ammonia
chemistry.chemical_compound
Nickel
Colloid and Surface Chemistry
Adsorption
chemistry
Reversible hydrogen electrode
Subjects
Details
- ISSN :
- 15205126
- Volume :
- 142
- Issue :
- 12
- Database :
- OpenAIRE
- Journal :
- Journal of the American Chemical Society
- Accession number :
- edsair.doi.dedup.....19494f69a301fa6df004e763579bc406