Enhanced Nitrate-to-Ammonia Activity on Copper-Nickel Alloys via Tuning of Intermediate Adsorption

Yuhang Wang, Aoni Xu, Ziyun Wang, Linsong Huang, Jun Li, Fengwang Li, Joshua Wicks, Mingchuan Luo, Dae Hyun Nam, Chih Shan Tan, Yu Ding, Jiawen Wu, Yanwei Lum, Cao Thang Dinh, David Sinton, Gengfeng Zheng, Edward H. Sargent*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

26 Scopus citations

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.

Original languageEnglish
Pages (from-to)5702-5708
Number of pages7
JournalJournal of the American Chemical Society
Volume142
Issue number12
DOIs
StatePublished - 25 Mar 2020

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