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Abatement of dichloromethane with high selectivity over defect-rich MOF-derived Ru/TiO 2 catalysts.

Shaohua ChaiShuangde LiLe ZhangGuijun FanLinfeng NieXin ZhouWuxinchen YangWeiman LiYunfa Chen
Published in: Nanoscale (2022)
The regulation of oxygen vacancies and Ru species using metal-organic frameworks was synergically adopted in a rational design to upgrade Ru/TiO 2 catalysts, which are highly active for the catalytic oxidation of dichloromethane (DCM) with less undesired byproducts. In this work, Ru/M-TiO 2 and Ru/N-TiO 2 catalysts were synthesized by the pyrolysis of MIL-125 and NH 2 -MIL-125 incorporated with Ru, the existence of Ru nanoclusters and nanoparticles was detected by XAFS, respectively, and the catalytic performance was analyzed comprehensively. Complete oxidation of DCM was obtained at ∼290 °C over Ru/M-TiO 2 and Ru/N-TiO 2 catalysts, while Ru/N-TiO 2 showed quite less monochloromethane (MCM) and higher CO 2 yields, and better dechlorination capacity in oxidation. The distinction comes down to that the easier desorption of chlorine could be achieved over Ru 4+ which act as the main activated adsorption sites for DCM in Ru/N-TiO 2 , compared to oxygen vacancies that serve as the main dissociation sites in Ru/M-TiO 2 . Additionally, Ru/N-TiO 2 exhibited superior stability and excellent resilience in moisture. An in situ DRIFTS experiment further indicated the different DCM catalytic degradation process as well as the reaction mechanism over the as-prepared catalysts.
Keyphrases
  • energy transfer
  • metal organic framework
  • quantum dots
  • visible light
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  • fluorescent probe