期刊
JOURNAL OF CHEMICAL PHYSICS
卷 150, 期 4, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.5048036
关键词
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资金
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Catalysis Science Program [DE-SC0016529]
- National Science Foundation [ACI-1053575]
- Computational Materials Education and Training (CoMET) NSF Research Traineeship [DGE-1449785]
Electrochemical ammonia synthesis could provide a sustainable and efficient alternative to the energy intensive Haber-Bosch process. Development of an active and selective N-2 electroreduction catalyst requires mechanism determination to aid in connecting the catalyst composition and structure to performance. Density functional theory (DFT) calculations are used to examine the elementary step energetics of associative N-2 reduction mechanisms on two low index Fe surfaces. Interfacial water molecules in the Heyrovsky-like mechanism help lower some of the elementary activation barriers. Electrode potential dependent barriers show that cathodic potentials below -1.5 V-RHE (reversible hydrogen electrode) are necessary to give a significant rate of N-2 electroreduction. DFT barriers suggest a larger overpotential than expected based on elementary reaction free energies. Linear Bronsted-Evans-Polanyi relationships do not hold across N-H formation steps on these surfaces, further confirming that explicit barriers should be considered in DFT studies of the nitrogen reduction reaction. Published under license by AIP Publishing.
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