Mutual Self-Regulation of d-Electrons of Single Atoms and Adjacent Nanoparticles for Bifunctional Oxygen Electrocatalysis and Rechargeable Zinc-Air Batteries

Highlights A new class of γ-cyclodextrin based metal–organic framework -derived strategy was used to fabricate highly active M–N-C catalysts containing both single-atom sites and nanoparticles. The obtained Co@C-CoNC exhibits remarkable bifunctional oxygen reduction (ORR)/oxygen evolution reactions (OER) performance, which further delivered a high power density and excellent cyclic stability in rechargeable zinc-air batteries. Density functional theory calculation suggests that the mutual self-regulation of d-electron density of both Co NP and Co SAC conjointly reduce the reaction energy barriers and thus boost the ORR/OER kinetics through their fast adsorption/desorption ability of reaction intermediates.