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Charge transfer dependence on CO2 hydrogenation activity to methanol in Cu nanoparticles covered with metal-organic framework systems.

Hirokazu KobayashiJared M TaylorYuko MitsukaNaoki OgiwaraTomokazu YamamotoTakaaki ToriyamaSyo MatsumuraHiroshi Kitagawa
Published in: Chemical science (2019)
We report the synthesis and characterization of highly active Cu nanoparticles covered with zirconium/hafnium-based metal-organic frameworks for CO2 hydrogenation to methanol. Compared to Cu/γ-Al2O3 , Cu/ZIF-8, Cu/MIL-100 and Cu/UiO-66 composites, UiO-66 acts as the most active support, with Cu/Zr-UiO-66 producing methanol at a rate 70 times higher than that of Cu/γ-Al2O3 . In addition, the replacement of Zr4+ with Hf4+ in UiO-66 tripled in the rate of methanol production. Furthermore, we describe a substituent effect on the catalytic activity, with Cu/Zr-UiO66-COOH providing a three-fold enhancement of methanol production, compared to that of Zr-UiO-66 or Zr-UiO66-NH2 . The enhanced catalytic activity of Cu nanoparticles depends on the charge transfer degree from Cu nanoparticles to UiO-66 at the interface between Cu nanoparticles and UiO-66.
Keyphrases
  • metal organic framework
  • pet imaging
  • heart failure
  • carbon dioxide
  • gold nanoparticles
  • mass spectrometry
  • aqueous solution
  • positron emission tomography