Pseudo-atomic-scale metals well-dispersed on nano-carbons as ultra-low metal loading oxygen-evolving electrocatalysts

Solving challenges for the scaling-up, high metal loadings and low turnover frequency (TOF, defined as mol O2 per mol metal per second), of FeNi catalysts in water electrolysis, we report the first discovery of pH tunable tannic acid single molecular layer formed on nano-sized carbons (NCs), which promotes the gram-production of pseudo-atomic-scale FeNi oxyhydroxide nanoclusters well-dispersed on NCs. It results in ultra-low metal loading (0.42 μg cm^-2) and remarkably large TOF of 14.03 s^-1 for the oxygen evolution reaction, which is three orders of magnitude higher than that of state-of-the-art FeNi catalysts. A "volcano"-shaped activity trend in specific activity and TOF was found to depend on the Fe content in FeNi oxyhydroxide. The micro-morphologies from the atomic-level exposure of active sites and surface spectra analyses confirm the model of synergism between Ni and Fe centers.