Approaching the activity limit of CoSe2 for oxygen evolution via Fe doping and Co vacancy

Abstract Electronic structure engineering lies at the heart of efficient catalyst design. Most previous studies, however, utilize only one technique to modulate the electronic structure, and therefore optimal electronic states are hard to be achieved. In this work, we incorporate both Fe dopants and Co vacancies into atomically thin CoSe 2 nanobelts for /coxygen evolution catalysis, and the resulted CoSe 2 -D Fe –V Co exhibits much higher catalytic activity than other defect-activated CoSe 2 and previously reported FeCo compounds. Deep characterizations and theoretical calculations identify the most active center of Co 2 site that is adjacent to the V Co -nearest surface Fe site. Fe doping and Co vacancy synergistically tune the electronic states of Co 2 to a near-optimal value, resulting in greatly decreased binding energy of OH* (ΔE OH ) without changing ΔE O , and consequently lowering the catalytic overpotential. The proper combination of multiple defect structures is promising to unlock the catalytic power of different catalysts for various electrochemical reactions.