3 years ago

Stability of residual oxides in oxide-derived Cu catalysts for electrochemical CO2 reduction investigated with 18O labeling

Yanwei Lum, Joel W. Ager
Oxide-derived (OD) Cu catalysts have high selectivity towards the formation of multi-carbon products (C2/C3) for aqueous electrochemical CO2 reduction (CO2R). It has been proposed that a large fraction of the initial oxide can be surprisingly resistant to reduction and that these residual oxides play a crucial role in promoting the formation of C2/C3 products. We investigate the stability of residual oxides by synthesizing 18O enriched OD Cu catalysts and testing them for CO2R. These catalysts maintain a high selectivity towards C2/C3 products (~60%) for up to 5h in 0.1 M KHCO3 at -1.0 V vs RHE. However, secondary ion mass spectrometry measurements show that only a small fraction (< 1%) of the original 18O content remains, showing that residual oxides are not present in significant amounts during CO2R. Furthermore, we show that OD Cu reoxidizes rapidly in the absence of a reducing potential, which could compromise the accuracy of ex-situ methods for determining the true oxygen content.

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/anie.201710590

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