Efficient conversion of low-concentration nitrate sources into ammonia on a Ru-dispersed Cu nanowire electrocatalyst

Chen, Feng-Yang; Wu, Zhen-Yu; Gupta, Srishti; Rivera, Daniel J.; Lambeets, Sten V.; Pecaut, Stephanie; Kim, Jung Yoon Timothy; Zhu, Peng; Finfrock, Y. Zou; Meira, Debora Motta; King, Graham; Gao, Guanhui; Xu, Wenqian; Cullen, David A.; Zhou, Hua; Han, Yimo; Perea, Daniel E.; Muhich, Christopher L.; Wang, Haotian

doi:10.1038/s41565-022-01121-4

Efficient conversion of low-concentration nitrate sources into ammonia on a Ru-dispersed Cu nanowire electrocatalyst

Journal Article · Mon May 02 00:00:00 EDT 2022 · Nature Nanotechnology

DOI:https://doi.org/10.1038/s41565-022-01121-4· OSTI ID:1883856

^[1]; ^[1]; ^[2]; ^[2]; ^[3]; ^[1]; ^[1]; ^[1]; Finfrock, Y. Zou ^[4]; Meira, Debora Motta ^[5]; ^[5]; Gao, Guanhui ^[1]; Xu, Wenqian ^[6]; ^[7]; ^[6]; Han, Yimo ^[1]; ^[3]; Muhich, Christopher L. ^[2]; ^[1]

Rice University, Houston, TX (United States)
Arizona State University, Tempe, AZ (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Canadian Light Source, Saskatoon (Canada)
Argonne National Lab. (ANL), Lemont, IL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

We report electrochemically converting nitrate ions, a widely distributed nitrogen source in industrial wastewater and polluted groundwater, into ammonia represents a sustainable route for both wastewater treatment and ammonia generation. However, it is currently hindered by low catalytic activities, especially under low nitrate concentrations. Here we report a high-performance Ru-dispersed Cu nanowire catalyst that delivers an industrial-relevant nitrate reduction current of 1 A cm^–2 while maintaining a high NH₃ Faradaic efficiency of 93%. More importantly, this high nitrate-reduction catalytic activity enables over a 99% nitrate conversion into ammonia, from an industrial wastewater level of 2,000 ppm to a drinkable water level <50 ppm, while still maintaining an over 90% Faradaic efficiency. Coupling the nitrate reduction effluent stream with an air stripping process, we successfully obtained high purity solid NH₄Cl and liquid NH₃ solution products, which suggests a practical approach to convert wastewater nitrate into valuable ammonia products. Density functional theory calculations reveal that the highly dispersed Ru atoms provide active nitrate reduction sites and the surrounding Cu sites can suppress the main side reaction, the hydrogen evolution reaction.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Lemont, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: Canada Foundation for Innovation (CFI); Canadian Institutes of Health Research (CIHR); National Research Council (Canada); National Research Council (NRC); National Science Foundation; National Science Foundation (NSF); Natural Sciences and Engineering Research Council (NSERC); Natural Sciences and Engineering Research Council of Canada (NSERC); Oak Ridge National Laboratory (ORNL); Rice University; USDOE Office of Science (SC), Biological and Environmental Research (BER); University of Saskatchewan; Welch Foundation

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725; AC05-76RL01830

OSTI ID:: 1883856

Alternate ID(s):: OSTI ID: 1991344

Journal Information:: Nature Nanotechnology, Journal Name: Nature Nanotechnology Journal Issue: 7 Vol. 17; ISSN 1748-3387

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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