Surface-Exposed Single-Ni Atoms with Potential-Driven Dynamic Behaviors for Highly Efficient Electrocatalytic Oxygen Evolution

Trapping the active sites on the exterior surface of hollow supports can reduce mass transfer resistance and enhance atomic utilization. Herein, we report a facile chemical vapor deposition strategy to synthesize single-Ni atoms decorated hollow S/N-doped football-like carbon spheres (Ni SAs@S/N-FCS). Specifically, the CdS@3-aminophenol/formaldehyde is carbonized into S/N-FCS. The gas-migrated Ni species are anchored on the surface of S/N-FCS simultaneously, yielding Ni SAs@S/N-FCS. The obtained catalyst exhibits outstanding performance for alkaline oxygen evolution reaction (OER) with an overpotential of 249 mV at 10 mA cm⁻², a small Tafel slope of 56.5 mV dec⁻¹, and ultra-long stability up to 166 hours without obvious fading. Moreover, the potential-driven dynamic behaviors of Ni-N₄ sites and the contribution of the S dopant at different locations in the matrix to the OER activity are revealed by the operando X-ray absorption spectroscopy and theoretical calculations, respectively. © 2022 Wiley-VCH GmbH.