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  • Title: Symmetry-Breaking p-Block Antimony Single Atoms Trigger N-Bridged Titanium Sites for Electrocatalytic Nitrogen Reduction with High Efficiency.
    Author: Gu H, Li J, Niu X, Lin J, Chen LW, Zhang Z, Shi Z, Sun Z, Liu Q, Zhang P, Yan W, Wang Y, Zhang L, Li P, Li X, Wang D, Yin P, Chen W.
    Journal: ACS Nano; 2023 Nov 14; 17(21):21838-21849. PubMed ID: 37909679.
    Abstract:
    The electrochemical nitrogen reduction reaction (eNRR) under mild conditions emerges as a promising approach to produce ammonia (NH3) compared to the typical Haber-Bosch process. Herein, we design an asymmetrically coordinated p-block antimony single-atom catalyst immobilized on nitrogen-doped Ti3C2Tx (Sb SA/N-Ti3C2Tx) for eNRR, which exhibits ultrahigh NH3 yield (108.3 μg h-1 mgcat-1) and excellent Faradaic efficiency (41.2%) at -0.3 V vs RHE. Complementary in situ spectroscopies with theoretical calculations reveal that the nitrogen-bridged two titanium atoms triggered by an adjacent asymmetrical Sb-N1C2 moiety act as the active sites for facilitating the protonation of the rate-determining step from *N2 to *N2H and the kinetic conversion of key intermediates during eNRR. Moreover, the introduction of Sb-N1C2 promotes the formation of oxygen vacancies to expose more titanium sites. This work presents a strategy for single-atom-decorated ultrathin two-dimensional materials with the aim of simultaneously enhancing NH3 yield and Faradaic efficiency for electrocatalytic nitrogen reduction.
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