Photoactive Zeolitic Imidazolate Framework as Intrinsic Heterogeneous Catalysts for Light-Driven Hydrogen Generation
Abstract
Zeolitic imidazolate frameworks (ZIFs) with intrinsic photoactivity represent an excellent scaffold for a single-site photocatalytic center. However, their application in visible-light-driven photocatalysis is hampered by their light-harvesting ability due to limited coverage in the realm of the solar spectrum and relatively low extinction coefficient. In this work, we report the first example of the enhanced light-harvesting property of ZIF-67 via energy transfer from a molecular photosensitizer, that is, the RuN3 complex, sensitized on the surface of ZIF-67. Using transient absorption spectroscopy, we show that energy transfer occurs from the excited RuN3 to ZIF-67 with ~86.9% efficiency. More importantly, this RuN3/ZIF-67 hybrid system exhibits significantly enhanced photocatalytic activity for H2 production from water, which can be attributed to efficient energy transfer from RuN3.
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1351376
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Energy Letters
- Additional Journal Information:
- Journal Volume: 2; Journal Issue: 1; Journal ID: ISSN 2380-8195
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- ENGLISH
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Thin films; Photocatalysis; Absorption; Physical and chemical processes; Kinetics
Citation Formats
Yang, Sizhuo, Pattengale, Brian, Kovrigin, Evgenii L., and Huang, Jier. Photoactive Zeolitic Imidazolate Framework as Intrinsic Heterogeneous Catalysts for Light-Driven Hydrogen Generation. United States: N. p., 2016.
Web. doi:10.1021/acsenergylett.6b00540.
Yang, Sizhuo, Pattengale, Brian, Kovrigin, Evgenii L., & Huang, Jier. Photoactive Zeolitic Imidazolate Framework as Intrinsic Heterogeneous Catalysts for Light-Driven Hydrogen Generation. United States. https://doi.org/10.1021/acsenergylett.6b00540
Yang, Sizhuo, Pattengale, Brian, Kovrigin, Evgenii L., and Huang, Jier. Fri .
"Photoactive Zeolitic Imidazolate Framework as Intrinsic Heterogeneous Catalysts for Light-Driven Hydrogen Generation". United States. https://doi.org/10.1021/acsenergylett.6b00540. https://www.osti.gov/servlets/purl/1351376.
@article{osti_1351376,
title = {Photoactive Zeolitic Imidazolate Framework as Intrinsic Heterogeneous Catalysts for Light-Driven Hydrogen Generation},
author = {Yang, Sizhuo and Pattengale, Brian and Kovrigin, Evgenii L. and Huang, Jier},
abstractNote = {Zeolitic imidazolate frameworks (ZIFs) with intrinsic photoactivity represent an excellent scaffold for a single-site photocatalytic center. However, their application in visible-light-driven photocatalysis is hampered by their light-harvesting ability due to limited coverage in the realm of the solar spectrum and relatively low extinction coefficient. In this work, we report the first example of the enhanced light-harvesting property of ZIF-67 via energy transfer from a molecular photosensitizer, that is, the RuN3 complex, sensitized on the surface of ZIF-67. Using transient absorption spectroscopy, we show that energy transfer occurs from the excited RuN3 to ZIF-67 with ~86.9% efficiency. More importantly, this RuN3/ZIF-67 hybrid system exhibits significantly enhanced photocatalytic activity for H2 production from water, which can be attributed to efficient energy transfer from RuN3.},
doi = {10.1021/acsenergylett.6b00540},
journal = {ACS Energy Letters},
number = 1,
volume = 2,
place = {United States},
year = {Fri Dec 09 00:00:00 EST 2016},
month = {Fri Dec 09 00:00:00 EST 2016}
}
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Figures / Tables:
Figure 1: (a) UV-visible absorption spectra of ZIF-67, RuN3/ZIF-67, and RuN3/Al2O3 thin films. The inset shows the spectral overlap between the absorption spectrum of ZIF-67 and emission spectrum of RuN3. (b) Powder XRD patterns of ZIF-67 and RuN3/ZIF-67. The inset shows the cartoon of RuN3 sensitized ZIF-67. The yellow ballmore »
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