Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.088
Publication date: 18th July 2019
Synergistic effects at metal/metal oxide interfaces have been associated with highly active and selective catalytic motifs. So far, such interactions have been rarely explored to enhance the selectivity in the electrochemical CO2 reduction reaction. Herein, we discuss our recent work on Cu/CeO2-x heterodimers (HDs) which highlights the beneficial effects of such interface towards promoting the electrochemical CO2 reduction reaction (CO2RR) [1]. We have developed a colloidal seeded-growth synthesis to connect the two highly mismatched domains (Cu and CeO2-x) and to tune the extension of the interface by varying the size of the Cu domain. The Cu/CeO2-x HDs exhibit state-of-the-art selectivity towards CO2RR (up to ~80%) against the competitive hydrogen evolution reaction (HER) and high faradaic efficiency for methane (up to ~54%) at -1.2 VRHE, which is ~5 times higher than that obtained when the Cu and CeO2-x nanocrystals are physically mixed. Operando X-Ray absorption spectroscopy along with other ex-situ spectroscopies evidences the partial reduction from Ce4+ to Ce3+ in the HDs during CO2RR. The DFT study of the active site motif in reducing condition proposed that lowest free energy pathway utilizes O-vacancy site with intermediates binding to both Cu and Ce atoms, a configuration which allows to break the CHO*/CO* scaling relation. Within this concept, other metal oxides are under investigation to demonstrate the influence of support in the catalytic properties of Cu-metal oxide interface.
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