Step-Edge Functionalization by N-Heterocyclic Carbenes Enhances Catalytic Activity in Electrochemical CO2 Reduction.

Wiesener P; Das A; Kolodzeiski E; Tran D; Pan Y; Fuchs H; López-Salas N; Amirjalayer S; Glorius F; Mönig H

Abstract

reduction compared to undecorated metallic step-edges. Using high-resolution scanning probe microscopy, an upright-tilted adsorption geometry and a unified binding mode of three different NHCs at step-edges are revealed. The exceptional stability of these well-defined nanostructures allows the use of the single-crystalline samples as working electrodes in electrochemical experiments. Photoelectron spectroscopy and theoretical simulations correlate charge transfer and conformational details with their catalytic performance. By combining macroscopic electrochemical experiments with single-molecule microscopy, this study highlights NHC step-edge functionalization as an effective approach to design highly selective and efficient catalysts.