Abstract
The direct correlation between active sites and catalytic activity in multiple-component metal-organic frameworks (MOFs) is key to understanding their mechanism of oxygen evolution reaction (OER) but remains vague. Herein, supported multiple-site MOFs are adopted as model catalysts to quantitatively study the composition-dependent OER performance. Ni MOFs on Fe metal substrate possess the highest intrinsic OER activity with the Ni/Fe ratio of 1:2 in the presence of metal leaching of the substrate during synthesis. Further introducing a proper amount of Cu further boosts the OER performance of Cu-doped NiFe MOFs with an impressively low overpotential of 200 mV at 10 mA cm−2. Spectroscopic analysis with theoretical study indicates that the copper doping within the NiFe MOFs induces electron redistribution for high valence Fe sites with an optimized balance of OH/OOH adsorption and decreased energy barrier for improved OER. This work sheds light on the active site tailoring of MOFs which highly correlates with the OER activity.