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  • Title: Microwave Regenerable Nickel, Zinc Co-doped Nitrogen-Coordinated Porous Carbon Catalyst for Nitrogen Fixation.
    Author: Deng P, Liu Y, Liu Y, Li Y, Wu R, Meng L, Liang K, Gan Y, Qiao F, Liu N, Kang Z, Li H.
    Journal: ACS Appl Mater Interfaces; 2023 Sep 27; 15(38):44809-44819. PubMed ID: 37698442.
    Abstract:
    More than 90% of the global NH3 synthesis is dominated by the Haber-Bosch process, which consumes 2% of the worldwide energy and generates 1.44% of the global carbon emission. The electrochemical N2 reduction reaction (NRR) is regarded as an attractive alternative route to produce NH3 under mild reaction conditions, but the electrocatalysts suffer from the difficulty of N≡N cleavage. In this work, we report a leaf-like MOF-derived Ni/Zn bimetallic co-doped nitrogen-coordinated porous carbon (Ni/Zn-NPC) as a cost-effective NH3 synthesis electrocatalyst. The resultant electrocatalyst achieved a high NH3 production rate of 22.68 μg h-1 mgcat-1 at -1.0 V vs a reversible hydrogen electrode (RHE) in a 0.1 M Na2SO4 electrolyte. The Ni/Zn-NPC material can be called a microwave regenerable catalyst because microwave treatment has proven to be a crucial part of the multi-field coupling to detoxify and make the catalyst reactive, further improving its stability. Density functional theory (DFT) was chosen to explore the mechanism of Ni/Zn-NPC for NRR, providing a profound prediction of the structure of the active site and related reaction pathways and revealing that trace Ni doping optimizes the local coordination environment and N2 adsorption of Zn atoms.
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