Publication date: 7th June 2020
Synergistic effects at metal/metal oxide interfaces often give rise to highly active and selective catalytic motifs, but were rarely explored for electrochemical CO2 reduction reaction (eCO2RR). Herein, Cu/CeO2-x hybrid nanocrystals (HNCs) are synthesized and presented as one of the prime examples where such effects promote eCO2RR. A colloidal seeded-growth synthesis is developed to connect the two highly mismatched domains through tunable no. of interfaces. Cu/(CeO2-x)1 HNCs exhibit a supreme selectivity towards eCO2RR (up to ~80%) against the competitive hydrogen evolution reaction (HER) and high faradaic efficiency for CH4 (up to ~54%) at -1.2 VRHE, which is ~5 times higher than that when the Cu and CeO2-x NCs are physically mixed. Operando X-ray absorption spectroscopy along with other ex-situ spectroscopies evidences that the level of partial reduction from Ce4+ to Ce3+ in HNCs decreases with the following order, Cu/(CeO2-x)1> Cu/(CeO2-x)2 > Cu/(CeO2-x)6, during CO2RR.
This work was primarily financed by the European Research Council under Starting Grant ERC-HYCAT with agreement number 715634. D.S. is supported by the Sandoz foundation.