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

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 d...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2023-06, Vol.62 (23), p.e202302253-n/a
Main Authors: Ning, Shangbo, Ou, Honghui, Li, Yaguang, Lv, Cuncai, Wang, Shufang, Wang, Dingsheng, Ye, Jinhua
Format: Article
Language:English
Subjects:
Alkenes
Amine oxidase (flavin-containing)
Carbon dioxide
Co0−Coδ+ Double Site
CO2 Hydrogenation
Cobalt oxides
Coupling
C−C Coupling
Hydrocarbons
Intermediates
Irradiation
Light irradiation
Light Olefins
Organic carbon
Paraffin
Photothermal conversion
Photothermocatalysis
Radiation
Total organic carbon
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Summary: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 MgAl2O4 (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. Co0−Coδ+ interfacial double sites exhibit excellent selectivity toward light olefins during the hydrogenation of CO2 enhanced by light irradiation when compared with pure metallic Co. Owing to the interfacial effect, Co0−Coδ+ exhibits a lower hydrogenation ability than metallic Co, tuning a pathway with a manageable activation barrier for C−C coupling.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202302253