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  • Title: Repairable body-centered cubic Fe0 anchoring on porous hollow nitrogen-doped carbon spheres with adjusting electron distribution for efficient electrocatalytic ammonia synthesis.
    Author: Qiao H, Yu Y, Xu X, Hao R, Zheng Z, Wen B, Huang H, Hu J.
    Journal: J Colloid Interface Sci; 2024 Nov; 673():537-549. PubMed ID: 38885539.
    Abstract:
    Electrocatalytic nitrogen reduction reaction (ENRR) is a promising and efficient method for ammonia production. However, ENRR is restricted by the adsorption and activation of N2. Herein, an efficient nitrogen reduction reaction (NRR) electrocatalyst loaded with zero valent iron (ZVI) particles onto porous nitrogen-doped carbon (NC) hollow spheres is reported. The optimal Fe@10N3C-950 exhibits excellent performance with high ammonia (NH3) yield (152.28 µg h-1 mgcat-1) and Faradaic efficiency (FE, 54.55 %) at - 0.3 V (versus reversible hydrogen electrode, vs. RHE). Bader charge shows that the adsorbed N2 acquires more electrons from Fe sites with body-centered cubic (BCC) structure to better activate N2. Moreover, i-t experiments are performed before electrocatalytic NH3 production to effectively eliminate the effect of oxidation on ZVI and thus, maintain high ENRR activity for Fe@10N3C-950. Theoretical calculations indicate that nitrogen doping not only reduces the Gibbs free energy of rate determining step (RDS), but the BCC-structured Fe can also decrease the energy barriers of N2 activation and RDS.
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