Pulsed Laser Confinement of Single Atomic Catalysts on Carbon Nanotube Matrix for Enhanced Oxygen Evolution Reaction

The design of atomically dispersed single atom catalysts (SACs) must consider high metal-atom loading amount, effective confinement, and strong interactions with matrix, which can maximize their catalytic performance. Here reported is a promising method to synthesize SACs on highly conductive multiwall carbon nanotube (MWCNT) supports using pulsed laser confinement (PLC) process in liquid. Atomic cobalt (Co) and phosphorus (P) with a high loading density are homogeneously incorporated on the outer wall of the MWCNT (Co–P SAC MWCNT). Density functional theory (DFT) calculations in combination with systematic control experiments found that the incorporated Co and P adatoms act as an adsorption energy optimizer and a charge transfer promoter, respectively. Hence, favorable kinetics and thermodynamics in Co–P SAC MWCNT can be simultaneously achieved for water oxidation resulting in a superior catalytic performance than the benchmark RuO2 catalyst. Crucially, total processing time for assembling Co–P SAC MWCNT via PLC process is less than 60 min, shedding light on the promising practical applications of our SAC design strategy.