A cage-based metal-organic framework (Ni-NKU-101) with biphenyl-3,3',5,5'-tetracarboxylic acid was synthesized via solvothermal method. Ni-NKU-101 contains two types of cages based on trinuclear and octa-nuclear nickel-clusters that are connected with each other by the 4-connected ligands, to form a 3D framework with a new topology. A mixed-metal strategy was used to synthesize isostructural bimetallic MOFs of Mx Ni1-x -NKU-101 (M=Mn, Co, Cu, Zn). The electrocatalytic studies showed that the hydrogen evolution reaction (HER) activity of Cux Ni1-x -NKU-101 is much higher than that of other Mx Ni1-x -NKU-101 catalysts in acidic aqueous solution, owing to the synergistic effect of the bimetallic centers. The optimized Cu0.19 Ni0.81 -NKU-101 has an overpotential of 324 mV at 10 mA cm-2 and a Tafel slope of 131 mV dec-1 . The mechanism of HER activity over these bimetallic MOF-based electrocatalysts are discussed in detail.
Keywords: electrocatalysts; hydrogen evolution reaction; metal-organic frameworks; mixed-metal strategy; synergistic effect.
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