Abstract
The coordination environment of Ru centers determines their catalytic performance, however, much less attention is focused on cluster-induced charge transfer in a Ru single-atom system. Herein, by density functional theory (DFT) calculations, a competitive coordination-pairing between Ru clusters (RuRu bond) and single-atoms (RuO bond) is revealed leading to the charge redistribution between Ru and O atoms in ZnFe2 O4 units which share more free electrons to participate in the hydrogen desorption process, optimizing the proton adsorption and hydrogen desorption. Thus, a clicking confinement strategy for building a competitive coordination-pairing between Ru clusters and single-atoms anchored on ZnFe2 Ox nanosheets over carbon via RuO ligand (Ru1, n -ZnFe2 Ox -C) is proposed. Benefiting from the optimized coordination effect and the electronic synergy between Ru clusters and single-atoms, such a catalyst demonstrates the excellent activity and excellent stability in alkaline and seawater media, which has exceptional hydrogen evolution reactionactivity with overpotentials as low as 10.1 and 15.9mV to reach the current density of 10mA cm-2 in alkaline and seawater media, respectively, higher than that of commercial Pt/C catalysts as a benchmark. Furthermore, it owns remarkably outstanding mass activity, approximately 2 and 8 times higher than that of Pt catalysts in alkaline and seawater media, respectively.
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