Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 8, Issue 12, Pages 6034-6040Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ta14005k
Keywords
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Funding
- Key Project of Chinese National Programs for Research and Development [2016YFC0203800]
- National Natural Science Foundation of China [51578288]
- Jiangsu Province Scientific and Technological Achievements into a Special Fund Project [BA2016055, BA2017095]
- Jiangsu Province Scientific and Technological Project [BK20180449]
- Top-notch Academic Programs Project of Jiangsu Higher Education Institutions
- Priority Academic Program Development of Jiangsu Higher Education Institutions
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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 pi-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 mu mol 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.
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