Ligand-modified nanoparticle surfaces influence CO electroreduction selectivity.

ABSTRACT: Improving the kinetics and selectivity of CO₂/CO electroreduction to valuable multi-carbon products is a challenge for science and is a requirement for practical relevance. Here we develop a thiol-modified surface ligand strategy that promotes electrochemical CO-to-acetate. We explore a picture wherein nucleophilic interaction between the lone pairs of sulfur and the empty orbitals of reaction intermediates contributes to making the acetate pathway more energetically accessible. Density functional theory calculations and Raman spectroscopy suggest a mechanism where the nucleophilic interaction increases the sp² hybridization of CO_(ad), facilitating the rate-determining step, CO* to (CHO)*. We find that the ligands stabilize the (HOOC-CH₂)* interm

SUBMITTER: Shirzadi E 

PROVIDER: S-EPMC10998913 | biostudies-literature | 2024 Apr

REPOSITORIES: biostudies-literature