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

Hirokazu Kobayashi, Jared M. Taylor, Yuko Mitsuka, Naoki Ogiwara, Tomokazu Yamamoto, Takaaki Toriyama, Syo Matsumura, Hiroshi Kitagawa

Research output: Contribution to journalArticlepeer-review

21 Citations (Scopus)

Abstract

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.

Original languageEnglish
Pages (from-to)3289-3294
Number of pages6
JournalChemical Science
Volume10
Issue number11
DOIs
Publication statusPublished - 2019

All Science Journal Classification (ASJC) codes

  • Chemistry(all)

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