Exceptional catalytic activity of oxygen evolution reaction via two-dimensional graphene multilayer confined...

Oxygen evolution reaction (OER) plays a key role in many renewable energy technologies such as water splitting and metal-air batteries. Metal-organic frameworks (MOFs) are appealing to design efficient OER electrocatalysts, however, their intrinsic poor conductivity strongly hinders the activity. Here, we show a strategy to boost the OER activity of poor-conductive MOFs by confining them between graphene multilayers. The resultant NiFe-MOF//G gives a record-low overpotential of 106 mV to reach 10 mA cm^-2 and retains the activity over 150 h, which is in significant contrast to 399 mV of the pristine NiFe-MOF. We use X-ray absorption spectroscopy (XAS) and computations to demonstrate that the nanoconfinement from graphene multilayers not only forms highly reactive NiO₆-FeO₅ distorted octahedral species in MOF structure but also lowers limiting potential for water oxidation reaction. We also demonstrate that the strategy is applicable to other MOFs of different structures to largely enhance their electrocatalytic activities.