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- Title
Accessing parity-forbidden d-d transitions for photocatalytic CO<sub>2</sub> reduction driven by infrared light.
- Authors
Li, Xiaodong; Li, Li; Chen, Guangbo; Chu, Xingyuan; Liu, Xiaohui; Naisa, Chandrasekhar; Pohl, Darius; Löffler, Markus; Feng, Xinliang
- 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. This study demonstrates the effectiveness and generality of utilizing ultrathin Cu-based hydrotalcite-like hydroxy salts as catalysts for infrared light-driven CO2 reduction based on their d-d orbital transition mechanism.
- Subjects
PHOTOREDUCTION; TRANSITION metal complexes; CHARGE exchange; INFRARED spectroscopy; IRRADIATION; X-ray spectroscopy; X-ray absorption
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-39666-0