Time-Resolved In-Situ Surface-Enhanced Raman Spectroscopy (SERS) of CO2 Electrochemical Reduction on Cu
Hongyu An a, Longfei Wu a, Ward van der Stam a, Bert Weckhuysen a
a Inorganic Chemistry and Catalysis, Debye Institute for Nanomaterials Science, Utrecht University, Netherlands
Poster, Hongyu An, 025
Publication date: 7th June 2020

Electrochemical reduction of CO2 to value-added products is a promising means to counter greenhouse effect, as well as utilizing renewable energy. Fast time-resolved spectroscopic techniques are required to elucidate the details of surface intermediate reaction. In this presentation time-resolved surface enhanced Raman spectroscopy (TR-SERS) is successfully performed with a time resolution of 1.2 sec. Anodic treatment is crucial for achieving the high signal/noise ratio required for TR-SERS measurements, as well as boosting the faradaic efficiency for hydrocarbons (especially ethylene), suggesting“hot spots”for SERS signal enhancement and active sites for CO-CO coupling are both created during anodic treatment, and are highly correlated. The initial formation of and evolution of CO intermediates and their coupling are characterized by the time- and potential-dependent behaviour of their SERS signal. Linear CO at 2088 cm-1 or higher are more related to direct CO desorption, and a highly active CO intermediate at 2050 cm-1 is crucial in the CO-CO coupling that leads to ethylene formation. The results provide valuable insights into the mechanism of C2+ hydrocarbon formation during CO2 electrochemical reduction on Cu, and prove the great potential of TR-SERS in electrocatalysis.

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