Issue 12, 2020

In situ self-assembly of zirconium metal–organic frameworks onto ultrathin carbon nitride for enhanced visible light-driven conversion of CO2 to CO

Abstract

A series of Zr-porphyrin metal–organic framework (Zr-PMOF)/ultrathin g-C3N4 (UCN) (ZPUCN) heterostructure photocatalysts, as stable and efficient catalysts for the photoreduction of CO2, have been fabricated via a facile in situ hydrothermal self-assembly method. An interfacial interaction is formed due to hollow Zr-PMOF nanotubes being surrounded by 3D ultrathin g-C3N4 (UCN) and benefiting from the ultrathin and conjugated π-structure of UCN, the unsaturated metal atoms and organic ligands of Zr-PMOFs can covalently link to organic g-C3N4. The interaction provides a platform for UCN as a conductor to transfer e or as a donor to transfer e to Zr–O cluster active sites to catalyze CO2, substantially achieving the spatial separation of charge carriers and suppressing the photogenerated electron–hole (e–h+) pair recombination rate. Benefitting from the cooperative effects of the well-designed nanostructure and chemical grafting, in the absence of triethanolamine, cocatalysts and photosensitizers, the optimized ZPUCN hybrid not only exhibits a better CO evolution yield (5.05 μmol g−1 h−1), which is 2.2 times and 3.2 times higher than those of pure Zr-PMOFs and UCN, respectively, but also displays excellent stability after 96 h photocatalysis. Information about the mechanism is also elucidated from selected characterizations.

Graphical abstract: In situ self-assembly of zirconium metal–organic frameworks onto ultrathin carbon nitride for enhanced visible light-driven conversion of CO2 to CO

Supplementary files

Article information

Article type
Paper
Submitted
23 dec 2019
Accepted
26 feb 2020
First published
28 feb 2020

J. Mater. Chem. A, 2020,8, 6034-6040

In situ self-assembly of zirconium metal–organic frameworks onto ultrathin carbon nitride for enhanced visible light-driven conversion of CO2 to CO

Y. Wang, W. Zhen, Y. Zeng, S. Wan, H. Guo, S. Zhang and Q. Zhong, J. Mater. Chem. A, 2020, 8, 6034 DOI: 10.1039/C9TA14005K

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