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

Autor: Chen FY; Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USA., Wu ZY; Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USA., Gupta S; School for Engineering of Matter, Transport, & Energy, Chemical Engineering Program, Arizona State University, Tempe, AZ, USA., Rivera DJ; School for Engineering of Matter, Transport, & Energy, Chemical Engineering Program, Arizona State University, Tempe, AZ, USA., Lambeets SV; Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA, USA., Pecaut S; Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USA., Kim JYT; Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USA., Zhu P; Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USA., Finfrock YZ; Structural Biology Center, X-ray Science Division, Argonne National Laboratory, Lemont, IL, USA., Meira DM; Canadian Light Source, Saskatoon, Saskatchewan, Canada., King G; Canadian Light Source, Saskatoon, Saskatchewan, Canada., Gao G; Electron Microscope Center, Department of Materials Science and NanoEngineering, Rice University, Houston, TX, USA., Xu W; Advanced Photon Source, Argonne National Laboratory, Lemont, IL, USA., Cullen DA; Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, USA., Zhou H; Advanced Photon Source, Argonne National Laboratory, Lemont, IL, USA., Han Y; Department of Materials Science and NanoEngineering, Rice University, Houston, TX, USA., Perea DE; Environmental Molecular Sciences Laboratory, Earth and Biological Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA, USA. Daniel.Perea@pnnl.gov., Muhich CL; School for Engineering of Matter, Transport, & Energy, Chemical Engineering Program, Arizona State University, Tempe, AZ, USA. cmuhich@asu.edu.; School for Engineering of Matter, Transport, & Energy, Materials Science & Engineering Program, Arizona State University, Tempe, AZ, USA. cmuhich@asu.edu., Wang H; Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USA. htwang@rice.edu.; Department of Materials Science and NanoEngineering, Rice University, Houston, TX, USA. htwang@rice.edu.; Department of Chemistry, Rice University, Houston, TX, USA. htwang@rice.edu.
Jazyk: angličtina
Zdroj: Nature nanotechnology [Nat Nanotechnol] 2022 Jul; Vol. 17 (7), pp. 759-767. Date of Electronic Publication: 2022 May 02.
DOI: 10.1038/s41565-022-01121-4
Abstrakt: 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 NH 3 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 NH 4 Cl and liquid NH 3 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.
(© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)
Databáze: MEDLINE
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