Deciphering and Suppressing Over-Oxidized Nitrogen in Nickel-Catalyzed Urea Electrolysis
Dr. Jianan Li
National Engineering Laboratory for Industrial Wastewater Treatment, School of Resources and Environmental Engineering, State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China
These authors contributed equally to this work.
Search for more papers by this authorJili Li
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
These authors contributed equally to this work.
Search for more papers by this authorTao Liu
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Search for more papers by this authorLin Chen
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Search for more papers by this authorCorresponding Author
Prof. Yefei Li
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Key Laboratory of Computational Physical Science, Fudan University, Shanghai, 200438 China
Search for more papers by this authorProf. Hualin Wang
National Engineering Laboratory for Industrial Wastewater Treatment, School of Resources and Environmental Engineering, State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China
Search for more papers by this authorProf. Xiurong Chen
National Engineering Laboratory for Industrial Wastewater Treatment, School of Resources and Environmental Engineering, State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China
Search for more papers by this authorCorresponding Author
Assist. Prof. Ming Gong
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Search for more papers by this authorProf. Zhi-Pan Liu
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Key Laboratory of Computational Physical Science, Fudan University, Shanghai, 200438 China
Search for more papers by this authorCorresponding Author
Prof. Xuejing Yang
National Engineering Laboratory for Industrial Wastewater Treatment, School of Resources and Environmental Engineering, State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China
Search for more papers by this authorDr. Jianan Li
National Engineering Laboratory for Industrial Wastewater Treatment, School of Resources and Environmental Engineering, State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China
These authors contributed equally to this work.
Search for more papers by this authorJili Li
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
These authors contributed equally to this work.
Search for more papers by this authorTao Liu
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Search for more papers by this authorLin Chen
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Search for more papers by this authorCorresponding Author
Prof. Yefei Li
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Key Laboratory of Computational Physical Science, Fudan University, Shanghai, 200438 China
Search for more papers by this authorProf. Hualin Wang
National Engineering Laboratory for Industrial Wastewater Treatment, School of Resources and Environmental Engineering, State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China
Search for more papers by this authorProf. Xiurong Chen
National Engineering Laboratory for Industrial Wastewater Treatment, School of Resources and Environmental Engineering, State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China
Search for more papers by this authorCorresponding Author
Assist. Prof. Ming Gong
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Search for more papers by this authorProf. Zhi-Pan Liu
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438 China
Key Laboratory of Computational Physical Science, Fudan University, Shanghai, 200438 China
Search for more papers by this authorCorresponding Author
Prof. Xuejing Yang
National Engineering Laboratory for Industrial Wastewater Treatment, School of Resources and Environmental Engineering, State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China
Search for more papers by this authorAbstract
Urea electrolysis is a prospective technology for simultaneous H2 production and nitrogen suppression in the process of water being used for energy production. Its sustainability is currently founded on innocuous N2 products; however, we discovered that prevalent nickel-based catalysts could generally over-oxidize urea into NO2− products with ≈80 % Faradaic efficiencies, posing potential secondary hazards to the environment. Trace amounts of over-oxidized NO3− and N2O were also detected. Using 15N isotopes and urea analogues, we derived a nitrogen-fate network involving a NO2−-formation pathway via OH−-assisted C−N cleavage and two N2-formation pathways via intra- and intermolecular coupling. DFT calculations confirmed that C−N cleavage is energetically more favorable. Inspired by the mechanism, a polyaniline-coating strategy was developed to locally enrich urea for increasing N2 production by a factor of two. These findings provide complementary insights into the nitrogen fate in water–energy nexus systems.
Conflict of interest
The authors declare no conflict of interest.
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