Interfacial Electrochemistry of Catalyst-Coordinated Graphene Nanoribbons.

The immobilization of molecular electrocatalysts on conductive electrodes is an appealing strategy for enhancing their overall activity relative to those of analogous molecular compounds. In this study, we report on the interfacial electrochemistry of self-assembled two-dimensional nanosheets of graphene nanoribbons () and analogs containing a Rh-based hydrogen evolution reaction (HER) catalyst () immobilized on conductive electrodes. Proton-coupled electron transfer (PCET) taking place at N-centers of the nanoribbons was utilized as an indirect reporter of the interfacial electric fields experienced by the monolayer nanosheet located within the electric double layer.