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000596137 1001_ $$00000-0003-2716-0912$$aKarmakar, Sanchita$$b0
000596137 245__ $$aDeveloping post-modified Ce-MOF as a photocatalyst: a detail mechanistic insight into CO$_2$ reduction toward selective C2 product formation
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000596137 520__ $$aVisible light-driven C–C bond formation to produce C2-based liquid fuel selectively from CO$_2$ is of great interest and remains a challenging task due to uphill electron transfer kinetics. Herein, we have developed [Ru(bpy)$_2$]$^{2+}$-grafted UiO-66-bpydc Ce-MOFvia post-synthetic modification to harvest visible light based on MLCT $(RU_{d\pi}^{II} \to \pi_{bpy}^*)$ transition. The employment of Ru-grafted Ce-MOF facilitates fast electron transfer due to the vacant low-lying 4f orbital of Ce$^{IV}$, which was realized from ultrafast transient absorption (TA) spectroscopy, XANES, and in situ UV-vis spectroscopy. The synergistic effect of facile electron transfer and concomitant accommodation of two CO$_2$ molecules in the proximal defect-site in Ce$^{IV}$ leads to facile C–C bond formation via COOH* coupling to yield acetic acid. The catalytic assembly produces 1133 μmol g$^{−1}$ of acetic acid with an impressive rate of 128 μmol g$^{−1}$ h$^{−1}$, suppressing the formation of other C1-based carbonaceous products in water (with selectivity 99.5%, apparent quantum yield (AQY) = 0.93%). A detailed DFT calculation has been performed to understand the mechanistic pathway of C–C bond formation, and the generation of different surface-adsorbed intermediates was further supported by in situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy.
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000596137 7001_ $$00000-0002-8193-2816$$aBarman, Soumitra$$b1
000596137 7001_ $$0P:(DE-H253)PIP1098320$$aRahimi, Faruk Ahamed$$b2
000596137 7001_ $$0P:(DE-H253)PIP1098281$$aBiswas, Sandip$$b3
000596137 7001_ $$00000-0001-9976-7719$$aNath, Sukhendu$$b4
000596137 7001_ $$0P:(DE-H253)PIP1098153$$aMaji, Tapas Kumar$$b5$$eCorresponding author
000596137 773__ $$0PERI:(DE-600)2439879-2$$a10.1039/D2EE03755F$$gVol. 16, no. 5, p. 2187 - 2198$$n5$$p2187 - 2198$$tEnergy & environmental science$$v16$$x1754-5692$$y2023
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000596137 8564_ $$uhttps://bib-pubdb1.desy.de/record/596137/files/Revised%20Manuscript.pdf$$yPublished on 2023-03-17. Available in OpenAccess from 2024-03-17.
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