Abstract

Transition metal (TM)-based carbon hybrids have numerous applications in the field of regenerative electrochemical energy. The synergetic effects of high conductivity of carbon supports and abundant catalytic active sites in TMs make these hybrids promising oxygen evolution reaction (OER) electrocatalysts. However, strategies for modulating the catalytic active species in the above hybrids are limited despite being highly sought after. Furthermore, the exact roles of chemical species in the hybrids (e.g., N, C, or TM) mainly responsible for this high OER performance remain unknown. Herein, an innovative approach based on atomic layer deposition is developed to tune the true active species in Co nanoparticle/N-doped carbon nanotube (Co/N-CNT) hybrids. Specifically, the configuration predominantly promoting water oxidation in an alkaline medium is identified as pyridinic N-Co-C. Furthermore, a physicochemical intact interface between metallic Co nanoparticles and conductive N-CNTs is demonstrated to induce synergetic effects for accelerating charge transfer and enhancing electrocatalytic activity as well as stability in the hybrid catalysts. The optimized hybrid catalyst is revealed to exhibit outstanding alkaline OER activity and stability, outperforming RuO2 , a benchmark novel OER electrocatalyst.

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