4.8 Article

Oxygen-vacancy-mediated energy transfer for singlet oxygen generation by diketone-anchored MIL-125

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 292, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcatb.2021.120197

Keywords

Acetylacetone; Oxygen vacancy; Triplet energy transfer; Singlet oxygen; Metal-organic frameworks

Funding

  1. National Natural Science Foundation of China [21976083]
  2. Key Technologies Research and Development Program of the Ministry of Science and Technology of the People's Republic of China [2018YFC1802003, 2019YFC0408302]
  3. Natural Science Foundation of Jiangsu Province, China [BK20190322]

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The importance of singlet oxygen (1O2) in various applications has driven research on photocatalytic generation of 1O2 using metal-organic frameworks (MOFs). Despite limitations in visible-light absorption and charge carrier recombination, beta-diketone anchoring on MIL-125 was found to enhance energy transfer and improve the photocatalytic generation of 1O2. This study sheds light on the potential of visible-light-responsive MOFs for 1O2 generation and suggests a new strategy for designing MOF-based photocatalysts.
The importance of singlet oxygen (1O2) in synthesis of fine chemicals, inactivation of viruses and bacteria, degradation of pollutants, and photodynamic therapy has promoted the research on photocatalytic generation of 1O2. Metal-organic frameworks (MOFs), owing to the tunable structure, are good candidate photocatalysts for 1O2 generation. However, due to the poor visible-light absorption capacity and the invalid recombination of charge carriers, the 1O2 generation yields of most MOFs are still limited. Here, we demonstrate that beta-diketone anchoring could improve the photocatalytic generation of 1O2 by MIL-125 through enhanced energy transfer. The enhanced energy transfer was attributed to both the narrowed bandgap and the diketone-derived oxygen vacancies, which function as the trapping sites for charge carriers. The results here shed light on the generation of 1O2 by visible-light-responsive MOFs and provide a new strategy for the design of MOFs-based photocatalysts.

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