Construction of superhydrophilic metal-organic frameworks with hierarchical microstructure for efficient overall water splitting

Metal-organic frameworks (MOFs) display promising potential due to their exquisite structural advantages. Carboxylate-based MOFs, such as MIL-53 structures, attract a lot of attention among MOF families because of their remarkable stability in water and even alkaline condition. Hence, the delicate hierarchical microstructure is constructed by introducing MoO42- into NH2-MIL-53(NiFe) using a straightforward solvothermal strategy. The NiFeMo-MOF/NF electrode manifests a superior OER performance, producing an overpotential of 239 mV at 50 mA cm-2 and a decent Tafel slope of 87.0 mV dec-1. Furthermore, in a typical electrodeposition equipment, NiFeMo-MOF/NF is applied as the working electrode and the composite electrode named as (M) Ni-NiOOH/NF is generated by electrodeposition and electrooxidation process to assess HER performance, producing an overpotential of 119 mV at 50 mA cm-2 and a decent Tafel slope of 58.3 mV dec-1. The integrated electrolysis device delivers an extraordinarily low cell voltage of 1.50 V at 10 mA cm-2 while applying NiFeMo-MOF/NF as the anode, (M)Ni-NiOOH/NF as the cathode for overall water splitting, exceeding the noble RuO2/NF||Pt-C/NF (1.60 V@10 mA cm-2). This study provides a promising design strategy for future electrolysis catalysts.