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  • Title: Selective NOx- Electroreduction to Ammonia on Isolated Ru Sites.
    Author: Ke Z, He D, Yan X, Hu W, Williams N, Kang H, Pan X, Huang J, Gu J, Xiao X.
    Journal: ACS Nano; 2023 Feb 28; 17(4):3483-3491. PubMed ID: 36745389.
    Abstract:
    Nitrate and nitrite (NOx-) are widespread contaminants in industrial wastewater and groundwater. Sustainable ammonia (NH3) production via NOx- electroreduction provides a prospective alternative to the energy-intensive industrialized Haber-Bosch process. However, selectively regulating the reaction pathway, which involves complicated electron/proton transfer, toward NH3 generation relies on the robust catalyst. A specific consideration in designing selective NOx--to-NH3 catalysts should meet the criteria to suppress competing hydrogen evolution and avoid the presence of neighboring active sites that are in favor of adverse N-N coupling. Nevertheless, efforts in this regard are still inadequate. Herein, we demonstrate that isolated ruthenium sites can selectively reduce NOx- into NH3, with maximal Faradaic efficiencies of 97.8% (NO2- reduction) and 72.8% (NO3- reduction) at -0.6 and -0.4 V, respectively. Density functional theory calculations simulated the reaction mechanisms and identified the *NO → *NOH as the potential rate-limiting step for NOx--to-NH3 conversion on single-atom Ru sites.
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