Porphyrin-based Ti-MOFs conferred with single-atom Pt for enhanced photocatalytic hydrogen evolution and NO removal

[Display omitted] •Uniformly distributed single-atom Pt with very high atomic utilization efficiency.•Unique Ti-oxo clusters as an alternative for the famous TiO2 photocatalyst.•Porphyrin units served as the linkers with a broad visible light-harvesting ability.•The catalyst could enhance hydrogen p...

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Veröffentlicht in:Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2022-01, Vol.428, p.132045, Article 132045
Hauptverfasser: Feng, Huan, Li, Houfan, Liu, Xingyan, Huang, Yumin, Pan, Qian, Peng, Rong, Du, Ruoyu, Zheng, Xuxu, Yin, Zhongyi, Li, Siqi, He, Youzhou
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Sprache:eng
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Zusammenfassung:[Display omitted] •Uniformly distributed single-atom Pt with very high atomic utilization efficiency.•Unique Ti-oxo clusters as an alternative for the famous TiO2 photocatalyst.•Porphyrin units served as the linkers with a broad visible light-harvesting ability.•The catalyst could enhance hydrogen production and NO elimination simultaneously.•The intermediates were analyzed by in-situ DRIFTS spectra during the NO removal. A robust and efficient titanium metal–organic framework (TMF-Pt) with a single-atom Pt embedded PtII tetrakis(4-carboxyphenyl)porphyrins (PtTCPP) as linking groups and Ti-oxo molecular clusters as metal nodes was successfully fabricated for the first time, which have been confirmed by aberration-correction scanning transmission electron microscopy (HAADF-STEM) and synchrotron-radiation-based X-ray absorption fine-structure spectroscopy (XAFS), and was applied to photocatalytic hydrogen production and NO removal. It was worth noting that the TMF-Pt exhibited an extremely high hydrogen evolution activity (15456 µmol·g−1·h−1) and NO removal rate (70.3%) in comparison with most of the reported MOFs-based photocatalysts, which could be ascribed to the very high atom-utilization efficiency of single-atom Pt along with a high charge carriers separation efficiency and the Ti-oxo clusters as an alternative to the very famous TiO2 photocatalyst. The results provided us with a novel strategy that introducing single-atom Pt into the center of the porphyrin skeleton could integrate the broad light-harvesting porphyrin unite with the very high atom-utilization efficiency single-atom Pt to further improve the photocatalytic performance ultimately.
ISSN:1385-8947
1873-3212
DOI:10.1016/j.cej.2021.132045