Abstract
AbstractElectronic metal–support interactions (EMSI) describe the electron flow between metal sites and a metal oxide support. It is generally used to follow the mechanism of redox reactions. In this study of CuO‐CeO2 redox, an additional flow of electrons from metallic Cu to surface carbon species is observed via a combination of operando X‐ray absorption spectroscopy, synchrotron X‐ray powder diffraction, near ambient pressure near edge X‐ray absorption fine structure spectroscopy, and diffuse reflectance infrared Fourier transform spectroscopy. An electronic metal–support–carbon interaction (EMSCI) is proposed to explain the reaction pathway of CO oxidation. The EMSCI provides a complete picture of the mass and electron flow, which will help predict and improve the catalytic performance in the selective activation of CO2, carbonate, or carbonyl species in C1 chemistry.
Highlights
The interaction between metals and supports plays a vital role in modulating the catalytic performance of active sites
The corresponding energy-dispersive X-ray spectroscopy (EDS) maps identify the presence of Cu in the form of ca. 5 nm particles surrounded by CeO2 (Figure S1a-e)
The surface Cu/(Cu + Ce) ratio determined by X-ray photoelectron spectroscopy (XPS) is 0.36, which is close to the theoretical bulk Cu/(Cu + Ce) ratio (0.35) for 20 wt % CuO-CeO2
Summary
The interaction between metals and supports plays a vital role in modulating the catalytic performance of active sites. The electrophilicity of surface carbon species is studied in an inert atmosphere (He stage) to exclude electron transfer from or to the gaseous molecules. The CO oxidation activity of the catalyst at individual stage is compared below 353 K to elucidate the impact of initial oxidation states of Cu and Ce as well as the surface carbon species. He Department of Materials Science and Engineering National University of Singapore Singapore, 117575 (Singapore). Angewandte Chemie International Edition published by Wiley-VCH GmbH
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