Electronic configuration regulation of single-atomic Mn sites mediated by Mo/Mn clusters for an efficient hydrogen evolution reaction

通过 Mo/Mn 团簇介导的单原子 Mn 位点电子构型调控实现高效析氢反应

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Abstract

Tuning the electron distribution of metal single-atom active sites via bimetallic clusters is an effective way to enhance their hydrogen evolution reaction (HER) activity, but remains a great challenge. A biochar-based electrocatalyst (BC(MoMn800-2)) with both MnN(4) active sites and Mo(2)C/Mn(7)C(3) clusters was synthesized using in situ enriched Mo/Mn biomass as a precursor to trigger the HER. Various characterization and density functional theory (DFT) calculation results indicated that the presence of Mo(2)C/Mn(7)C(3) clusters in BC(MoMn800-2) effectively induced the redistribution of charges at MnN(4) sites, reducing the energy of H* activation during the HER. In 0.5 M H(2)SO(4), the overpotential was 27.4 mV at a current density of 10 mA cm(-2) and the Tafel slope was 31 mV dec(-1), and its electrocatalytic performance was close to that of Pt/C. The electrocatalyst also exhibited excellent electrocatalytic stability and durability. This work might provide a new strategy for solid waste recycling and constructing efficient HER electrocatalysts.

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