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

Xiaodong Li, Li Li, Guangbo Chen, Xingyuan Chu, Xiaohui Liu, Chandrasekhar Naisa, Darius Pohl, Markus Löffler and Xinliang Feng ()
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Xiaodong Li: Max Planck Institute of Microstructure Physics, Weinberg 2
Li Li: University of Science and Technology of China
Guangbo Chen: Dresden University of Technology
Xingyuan Chu: Dresden University of Technology
Xiaohui Liu: Dresden University of Technology
Chandrasekhar Naisa: Dresden University of Technology
Darius Pohl: Dresden University of Technology, Helmholtzstreet
Markus Löffler: Dresden University of Technology, Helmholtzstreet
Xinliang Feng: Max Planck Institute of Microstructure Physics, Weinberg 2

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract A general approach to promote IR light-driven CO2 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, Cu4(SO4)(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 CO2 reduction, with a production rate of 21.95 and 4.11 μmol g−1 h−1 for CO and CH4, 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.

Date: 2023
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DOI: 10.1038/s41467-023-39666-0

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