Synergize curvature and confinement effects for Fe-, Co-, Ni- N2 sites on graphene nanobuds towards eNRR

Abstract

Exploring efficient and highly selective ammonia synthesis electrocatalysts can advance the development of both modern agriculture and industry. Graphene nanobuds (GN) feature both fullerene and graphene characteristics which inspires new design ideas of electrocatalysts for N2 reduction reaction (NRR) to ammonia based on the novel GN with traditional Fe-, Co-, Ni-N2 sites. Among these structures, CoN2-GN is investigated as the most promising candidate with a limiting potential of -0.83 V through a distal pathway. The excellent activity and selectivity for the eNRR can be attributed to synergistic effects originated from both confinement space of buds (fullerene fragment) and curvature of the junctions. Especially, acting as an H-activator to N2, the ‘neck’ C atoms in the GNs improve the selectivity significantly for eNRR and facilitate the subsequent processes. This research would greatly contribute to develop the novel, efficient, multi-component graphene-based eNRR catalysts.