Utilizing High Coordination Diversity in Carbon Nanocone Supported Catalytic Single-Atom Sites for Screening of...

The hydrogen evolution reaction (HER) and the oxygen reduction reaction (ORR) are crucial in various energy conversion and storage technologies. Performances of catalysts are appreciably affected by the adsorption energies of key reaction intermediates, whereas the active site engineering to achieve optimal adsorption energy remains challenging. Herein, using density functional theory calculations, we proposed a novel design of transition metal single-atom active sites supported by carbon nanocone (CNC) with high coordination diversity. The particularly diversified electronic states of CNC carbon atoms endow varying coordination to the metal active sites, which then results in a near-continuum distribution of adsorption energies for key intermediates. With this mode, 33 CNC-based active sites exhibit outstanding catalytic potential for the HER with near-zero free energy barriers. Meanwhile, five distinct Cu-N₃ active sites can serve as promising candidates for the ORR with low overpotentials. Our work suggests a new strategy of making nanocone-based single-atom catalysts with promising catalytic performance.