Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 6, Issue 24, Pages 11337-11345Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8ta02962h
Keywords
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Funding
- NSFC [21771197, 21720102007]
- STP Project of Guangzhou [201504010031]
- NSF of Guangdong Province [S2013030013474]
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Electron-deficient Ru/Rh half-sandwich units are optoelectronical, stereochemical, and redox and catalytically active in nature. Four different species of these units were designed and successfully incorporated into UiO-67 frameworks by post-synthetic exchange (PSE) method and employed for photocatalytic H-2 evolution and CO2 reduction. Among them, the PSE-MOF catalysts containing [M-OH2] (M = Rh or Ru) groups show higher photocatalytic activity than those with [M-Cl], providing a new example of the exploitation of H2O molecules as small ancillary ligands for the construction of Ru/Rh half-sandwich units and subsequent incorporation into MOFs as photocatalytic centers. The application of TEOA (triethanolamine) and DMA (N,N-dimethylaniline) as sacrificial agents leads to different catalytic mechanisms and durations. A long-term hydrogen evolution lasting for 174 h without significant decrease in efficiency was achieved in the RhOH2@UiO-DMA system, showing the advantage of PSE-MOFs as highly stable photocatalytic platforms with superior self-protective properties.
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