Home > Publications database > Developing post-modified Ce-MOF as a photocatalyst: a detail mechanistic insight into CO$_2$ reduction toward selective C2 product formation > print

001     596137
005     20250724132226.0
024 7 _ |a 10.1039/D2EE03755F
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100 1 _ |a Karmakar, Sanchita
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245 _ _ |a Developing post-modified Ce-MOF as a photocatalyst: a detail mechanistic insight into CO$_2$ reduction toward selective C2 product formation
260 _ _ |a Cambridge
|c 2023
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336 7 _ |a ARTICLE
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520 _ _ |a Visible light-driven C–C bond formation to produce C2-based liquid fuel selectively from CO$_2$ is of great interest and remains a challenging task due to uphill electron transfer kinetics. Herein, we have developed [Ru(bpy)$_2$]$^{2+}$-grafted UiO-66-bpydc Ce-MOFvia post-synthetic modification to harvest visible light based on MLCT $(RU_{d\pi}^{II} \to \pi_{bpy}^*)$ transition. The employment of Ru-grafted Ce-MOF facilitates fast electron transfer due to the vacant low-lying 4f orbital of Ce$^{IV}$, which was realized from ultrafast transient absorption (TA) spectroscopy, XANES, and in situ UV-vis spectroscopy. The synergistic effect of facile electron transfer and concomitant accommodation of two CO$_2$ molecules in the proximal defect-site in Ce$^{IV}$ leads to facile C–C bond formation via COOH* coupling to yield acetic acid. The catalytic assembly produces 1133 μmol g$^{−1}$ of acetic acid with an impressive rate of 128 μmol g$^{−1}$ h$^{−1}$, suppressing the formation of other C1-based carbonaceous products in water (with selectivity 99.5%, apparent quantum yield (AQY) = 0.93%). A detailed DFT calculation has been performed to understand the mechanistic pathway of C–C bond formation, and the generation of different surface-adsorbed intermediates was further supported by in situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy.
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700 1 _ |a Barman, Soumitra
|0 0000-0002-8193-2816
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700 1 _ |a Rahimi, Faruk Ahamed
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700 1 _ |a Biswas, Sandip
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700 1 _ |a Nath, Sukhendu
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700 1 _ |a Maji, Tapas Kumar
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773 _ _ |a 10.1039/D2EE03755F
|g Vol. 16, no. 5, p. 2187 - 2198
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|t Energy & environmental science
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|y 2023
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856 4 _ |u https://pubs.rsc.org/en/content/articlepdf/2023/ee/d2ee03755f
856 4 _ |u https://bib-pubdb1.desy.de/record/596137/files/Developing%20post-modified%20Ce-MOF%20as%20a.pdf
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856 4 _ |u https://bib-pubdb1.desy.de/record/596137/files/Revised%20Manuscript.pdf
|y Published on 2023-03-17. Available in OpenAccess from 2024-03-17.
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