Abstract

AbstractCoordinatively unsaturated metal (CUM) sites in metal organic frameworks (MOFs) have demonstrated distinct catalytic activities, yet remain great challenges in their designing and engineering. Herein, a novel “Coordination Geometric Hindrance” approach based on ionic liquids (ILs) is proposed for defects construction in bimetallic MOF, of which the steric effect of competitively coordinated anions of imidazole ILs ([EMIM]X) enables the interference with the ordered growth of bimetallic NiFe‐MOFs. Specifically, the PF6− anion displays the strongest binding energy with metals Ni and Fe, accordingly, facilitates the formation of CUM sites in NiFe‐BTC/IL‐PF6. Taking both advantages of CUM defects and good intrinsic conductivity of IL, NiFe‐BTC/IL‐PF6 achieves a superior electrocatalytic performance in the oxygen evolution reaction (OER), with the overpotential as low as 210 mV at 10 mA cm−2, and the Tafel slope of 103 mV dec−1, thus, giving an 18‐fold larger TOF of the commercial OER catalyst of RuO2.

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