Synthesis of Cu/CeO2-x Nanocrystalline Heterodimers with Interfacial Active Sites To Promote CO2 Electroreduction

By S. Varandili, Jianfeng Huang, E. Oveisi, G. D. de Gregorio, M. Mensi, M. Strach, J. Vávra, C. Gadiyar, Arghya Bhowmik, R. Buonsanti. ACS Catalysis, 2019

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Synergistic effects at metal/metal oxide interfaces often give rise to highly active and selective catalytic motifs. So far, such interactions have been rarely explored to enhance the selectivity in the electrochemical CO2 reduction reaction (CO2RR). Herein, Cu/CeO2-x heterodimers (HDs) are synthesized and presented as one of the prime examples where such effects promote CO2RR. A colloidal seeded-growth synthesis is developed to connect the two highly mismatched domains (Cu and CeO2-x) through an interface. The Cu/CeO2-x HDs exhibit state-of-the-art selectivity toward 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 of Ce4+ to Ce3+ in the HDs during CO2RR. A Density Functional Theory (DFT) study of the...

Subfields: Catalysis, Renewable Energy, Sustainability and the Environment

View Paper: https://www.semanticscholar.org/paper/e956b9305141f2da2840be8f63b7fb6bd40b7a0d