We found a match
Your institution may have rights to this item. Sign in to continue.
- Title
Operando Raman spectroscopy uncovers hydroxide and CO species enhance ethanol selectivity during pulsed CO<sub>2</sub> electroreduction.
- Authors
Herzog, Antonia; Lopez Luna, Mauricio; Jeon, Hyo Sang; Rettenmaier, Clara; Grosse, Philipp; Bergmann, Arno; Roldan Cuenya, Beatriz
- Abstract
Pulsed CO2 electroreduction (CO2RR) 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 Cu2O nanocubes (~ 30 nm) during pulsed CO2RR 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 of Cu-Oad or CuOx/(OH)y species, impacting the kinetics of CO adsorption and boosting the ethanol selectivity. However, a too low OHad coverage following the formation of bulk-like Cu2O induces a significant increase in the C1 selectivity, while a too high OHad coverage poisons the surface for C-C coupling. Thus, we unveil the importance of co-adsorbed OH on the alcohol formation under CO2RR conditions and thereby, pave the way for improved catalyst design and operating conditions. Controlling the selectivity of the electroreduction of CO2 to value-added products is challenging. Here, authors use sub-second operando Raman spectroscopy to analyze Cu catalyst surfaces and discover the pivotal role of co-adsorbed OH and CO in enhancing ethanol selectivity.
- Subjects
RAMAN spectroscopy; ETHANOL; ELECTROLYTIC reduction; COUPLING reactions (Chemistry); ADSORPTION kinetics; TIME-resolved spectroscopy; COPPER; SERS spectroscopy
- Publication
Nature Communications, 2024, Vol 15, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-024-48052-3