Large-Scale, Bottom-Up Synthesis of Binary Metal-Organic Framework Nanosheets for Efficient Water Oxidation

Ultrathin metal-organic framework (MOF) nanosheets (NSs) offer potential for many applications, but the synthetic strategies are largely limited to top-down, low-yield exfoliation methods. Herein, Ni-M-MOF (M=Fe, Al, Co, Mn, Zn, and Cd) NSs are reported with a thickness of only several atomic layers, prepared by a large-scale, bottom-up solvothermal method. The solvent mixture of N,N-dimethylacetamide and water plays key role in controlling the formation of these two-dimensional MOF NSs. The MOF NSs can be directly used as efficient electrocatalysts for the oxygen evolution reaction, in which the Ni-Fe-MOF NSs deliver a current density of 10 mA cm^-2 at a low overpotential of 221 mV with a small Tafel slope of 56.0 mV dec^-1 , and exhibit excellent stability for at least 20 h without obvious activity decay. Density functional theory calculations on the energy barriers for OER occurring at different metal sites confirm that Fe is the active site for OER at Ni-Fe-MOF NSs.