TY - JOUR
T1 - Efficient conversion of low-concentration nitrate sources into ammonia on a Ru-dispersed Cu nanowire electrocatalyst
AU - Chen, Feng Yang
AU - Wu, Zhen Yu
AU - Gupta, Srishti
AU - Rivera, Daniel J.
AU - Lambeets, Sten V.
AU - Pecaut, Stephanie
AU - Kim, Jung Yoon Timothy
AU - Zhu, Peng
AU - Finfrock, Y. Zou
AU - Meira, Debora Motta
AU - King, Graham
AU - Gao, Guanhui
AU - Xu, Wenqian
AU - Cullen, David A.
AU - Zhou, Hua
AU - Han, Yimo
AU - Perea, Daniel E.
AU - Muhich, Christopher L.
AU - Wang, Haotian
N1 - Funding Information:
This work was supported by Rice University, the National Science Foundation Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT EEC 1449500) and a Welch Foundation Research Grant (C-2051-20200401). We acknowledge the use of the Electron Microscopy Center (EMC) at Rice University. Y.H. acknowledges the support from the Welch Foundation (C-2065-20210327). This research used resources of the Advanced Photon Source, a US Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by the Argonne National Laboratory under contract no. DE-AC02-06CH11357. A portion of this research was performed at the Environmental Molecular Sciences Laboratory, a DOE Office of Science User Facility sponsored by the Biological and Environmental Research program under Contract No. DE-AC05-76RL01830. Aberration-corrected STEM research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. Part of the research described in this article was performed at the Canadian Light Source, a national research facility of the University of Saskatchewan, which is supported by the Canada Foundation for Innovation (CFI), the Natural Sciences and Engineering Research Council (NSERC), the National Research Council (NRC), the Canadian Institutes of Health Research (CIHR), the Government of Saskatchewan and the University of Saskatchewan.
Publisher Copyright:
© 2022, The Author(s), under exclusive licence to Springer Nature Limited.
PY - 2022/7
Y1 - 2022/7
N2 - 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.
AB - 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.
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U2 - 10.1038/s41565-022-01121-4
DO - 10.1038/s41565-022-01121-4
M3 - Article
C2 - 35501378
AN - SCOPUS:85129312733
SN - 1748-3387
VL - 17
SP - 759
EP - 767
JO - Nature nanotechnology
JF - Nature nanotechnology
IS - 7
ER -