In this research, highly efficient heterogeneous bifunctional (BF) electrocatalysts (ECs) have been strategically designed by Fe coordination (C ) complexes, [Fe L (H O) Cl ] (C1) and [Fe L (H O) (SO )].2(CH O) (C2) where the high seven C number synergistically modifies the electronic environment of the Fe centre for facilitation of H O electrolysis. The electronic status of Fe and its adjacent atomic sites have been further modified by the replacement of -Cl in C1 by -SO in C2. Interestingly, compared to C1, the O-S-O bridged C2 reveals superior BF activity with extremely low overpotential (η) at 10 mA cm (140 mV , 62 mV ) and small Tafel slope (120.9 mV dec , 45.8 mV dec ). Additionally, C2 also facilitates a high-performance alkaline H O electrolyzer with cell voltage of 1.54 V at 10 mA cm and exhibits remarkable long-term stability. Thus, exploration of the intrinsic properties of metal-organic framework (MOF)-based ECs opens up a new approach to the rational design of a wide range of molecular catalysts.
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