Ru‐Doping Enhanced Electrocatalysis of Metal–Organic Framework Nanosheets toward Overall Water Splitting

Abstract An Ru‐doping strategy is reported to substantially improve both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) electrocatalytic activity of Ni/Fe‐based metal–organic framework (MOF) for overall water splitting. As‐synthesized Ru‐doped Ni/Fe MIL‐53 MOF nanosheets grown on nickel foam (MIL‐53(Ru‐NiFe)@NF) afford HER and OER current density of 50 mA cm −2 at an overpotential of 62 and 210 mV, respectively, in alkaline solution with a nominal Ru loading of ≈110 μg cm −2 . When using as both anodic and cathodic (pre‐)catalyst, MIL‐53(Ru‐NiFe)@NF enables overall water splitting at a current density of 50 mA cm −2 for a cell voltage of 1.6 V without iR compensation, which is much superior to state‐of‐the‐art RuO 2 ‐Pt/C‐based electrolyzer. It is discovered that the Ru‐doping considerably modulates the growth of MOF to form thin nanosheets, and enhances the intrinsic HER electrocatalytic activity by accelerating the sluggish Volmer step and improving the intermediate oxygen adsorption for increased OER catalytic activity.