Accessing parity-forbidden d-d transitions for photocatalytic CO2 reduction driven by infrared light

A general approach to promote IR light-driven CO 2 reduction within ultrathin Cu-based hydrotalcite-like hydroxy salts is presented. Associated band structures and optical properties of the Cu-based materials are first predicted by theory. Subsequently, Cu 4 (SO 4 )(OH) 6 nanosheets were synthesized...

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Bibliographic Details
Published in:Nature communications 2023-07, Vol.14 (1), p.4034-4034, Article 4034
Main Authors: Li, Xiaodong, Li, Li, Chen, Guangbo, Chu, Xingyuan, Liu, Xiaohui, Naisa, Chandrasekhar, Pohl, Darius, Löffler, Markus, Feng, Xinliang
Format: Article
Language:English
Subjects:
639/301/299/890
639/638/263
639/638/298
639/638/439/890
Absorption spectroscopy
Active sites
Carbon dioxide
Catalysts
Coordination compounds
Copper
Electron transfer
Fourier transforms
Humanities and Social Sciences
Infrared spectroscopy
Infrared tracking
Intermediates
Irradiation
Light
Light irradiation
Metal complexes
multidisciplinary
Optical properties
Photocatalysis
Science
Science (multidisciplinary)
Spectrum analysis
Transition metal compounds
X ray absorption
X-ray absorption spectroscopy
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Summary:A general approach to promote IR light-driven CO 2 reduction within ultrathin Cu-based hydrotalcite-like hydroxy salts is presented. Associated band structures and optical properties of the Cu-based materials are first predicted by theory. Subsequently, Cu 4 (SO 4 )(OH) 6 nanosheets were synthesized and are found to undergo cascaded electron transfer processes based on d - d orbital transitions under infrared light irradiation. The obtained samples exhibit excellent activity for IR light-driven CO 2 reduction, with a production rate of 21.95 and 4.11 μmol g −1 h −1 for CO and CH 4 , respectively, surpassing most reported catalysts under the same reaction conditions. X-ray absorption spectroscopy and in situ Fourier-transform infrared spectroscopy are used to track the evolution of the catalytic sites and intermediates to understand the photocatalytic mechanism. Similar ultrathin catalysts are also investigated to explore the generality of the proposed electron transfer approach. Our findings illustrate that abundant transition metal complexes hold great promise for IR light-responsive photocatalysis. This study demonstrates the effectiveness and generality of utilizing ultrathin Cu-based hydrotalcite-like hydroxy salts as catalysts for infrared light-driven CO 2 reduction based on their d-d orbital transition mechanism.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-023-39666-0