articleNature CommunicationsMay 11, 2024GOLD OA

Operando Raman spectroscopy uncovers hydroxide and CO species enhance ethanol selectivity during pulsed CO2 electroreduction

Fritz Haber Institute of the Max Planck Society · Massachusetts Institute of Technology · +2 more institutions

PubMed
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Abstract

Abstract Pulsed CO 2 electroreduction (CO 2 RR) has recently emerged as a facile way to in situ tune the product selectivity, in particular toward ethanol, without re-designing the catalytic system. However, in-depth mechanistic understanding requires comprehensive operando time-resolved studies to identify the kinetics and dynamics of the electrocatalytic interface. Here, we track the adsorbates and the catalyst state of pre-reduced Cu 2 O nanocubes ( ~ 30 nm) during pulsed CO 2 RR using sub-second time-resolved operando Raman spectroscopy. By screening a variety of product-steering pulse length conditions, we unravel the critical role of co-adsorbed OH and CO on the Cu surface next to the oxidative formation…

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