Guiding catalytic CO₂ reduction to ethanol with copper grain boundaries.

ABSTRACT: The grain boundaries (GBs) in copper (Cu) electrocatalysts have been suggested as active sites for CO₂ electroreduction to ethanol. Nevertheless, the mechanisms are still elusive. Herein, we describe how GBs tune the activity and selectivity for ethanol on two representative Cu-GB models, namely Cu∑3/(111) GB and Cu∑5/(100) GB, using joint first-principles calculations and experiments. The unique geometric structures on the GBs facilitate the adsorption of bidentate intermediates, *COOH and *CHO, which are crucial for CO₂ activation and CO protonation. The decreased CO-CHO coupling barriers on the GBs can be rationalized via kinetics analysis. Furthermore, when introducing GBs into Cu (100), the product is selectively switched from ethylene to ethanol, due to t

SUBMITTER: Cheng D 

PROVIDER: S-EPMC10370575 | biostudies-literature | 2023 Jul

REPOSITORIES: biostudies-literature