Co0 -Coδ+ Interface Double-Site-Mediated C-C Coupling for the Photothermal Conversion of CO2 into Light Olefins.

ABSTRACT

Solar-driven CO2 hydrogenation into multi-carbon products is a highly desirable, but challenging reaction. The bottleneck of this reaction lies in the C-C coupling of C1 intermediates. Herein, we construct the C-C coupling centre for C1 intermediates via the in situ formation of Co0 -Coδ+ interface double sites on MgAl2 O4 (Co-CoOx /MAO). Our experimental and theoretical prediction results confirmed the effective adsorption and activation of CO2 by the Co0 site to produce C1 intermediates, while the introduction of the electron-deficient state of Coδ+ can effectively reduce the energy barrier of the key CHCH* intermediates. Consequently, Co-CoOx /MAO exhibited a high C2-4 hydrocarbons production rate of 1303 µmol g-1 h-1 ; the total organic carbon selectivity of C2-4 hydrocarbons is 62.5 % under light irradiation with a high ratio (≈11) of olefin to paraffin. This study provides a new approach toward the design of photocatalysts used for CO2 conversion into C2+ products.