Volume 133, Issue 41 pp. 22457-22462
Zuschrift

Fabrication of Integrated Copper-Based Nanoparticles/Amorphous Metal–Organic Framework by a Facile Spray-Drying Method: Highly Enhanced CO2 Hydrogenation Activity for Methanol Synthesis

Yuko Mitsuka

Corresponding Author

Yuko Mitsuka

SHOEI CHEMICAL INC., 5-3, Aza-wakazakura, Fujinoki-machi, Tosu-shi Saga, 841-0048 Japan

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Dr. Naoki Ogiwara

Dr. Naoki Ogiwara

Division of Chemistry, Graduate School of Science, Kyoto University, Kitashirakawa-Oiwakecho, Sakyo-ku, Kyoto 606–8502 Japan

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Megumi Mukoyoshi

Megumi Mukoyoshi

Division of Chemistry, Graduate School of Science, Kyoto University, Kitashirakawa-Oiwakecho, Sakyo-ku, Kyoto 606–8502 Japan

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Prof. Hiroshi Kitagawa

Corresponding Author

Prof. Hiroshi Kitagawa

Division of Chemistry, Graduate School of Science, Kyoto University, Kitashirakawa-Oiwakecho, Sakyo-ku, Kyoto 606–8502 Japan

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Tomokazu Yamamoto

Tomokazu Yamamoto

Department of Applied Quantum Physics and Nuclear Engineering, Kyushu University, Motooka 744, Nishi-ku, Fukuoka, 819-0395 Japan

Kyushu University and the Ultramicroscopy Research Center, Motooka 744, Nishi-ku, Fukuoka, 819-0395 Japan

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Takaaki Toriyama

Takaaki Toriyama

Kyushu University and the Ultramicroscopy Research Center, Motooka 744, Nishi-ku, Fukuoka, 819-0395 Japan

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Prof. Syo Matsumura

Prof. Syo Matsumura

Department of Applied Quantum Physics and Nuclear Engineering, Kyushu University, Motooka 744, Nishi-ku, Fukuoka, 819-0395 Japan

Kyushu University and the Ultramicroscopy Research Center, Motooka 744, Nishi-ku, Fukuoka, 819-0395 Japan

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Prof. Masaaki Haneda

Prof. Masaaki Haneda

Advanced Ceramics Research Center, Nagoya Institute of Technology, 10-6-29 Asahigaoka, Tajimi, Gifu, 507-0071 Japan

Frontier Research Institute for Materials Science, Nagoya Institute of Technology, Gokiso-cho, Showaku, Nagoya, 465-8555 Japan

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Dr. Shogo Kawaguchi

Dr. Shogo Kawaguchi

Japan Synchrotron Radiation Research Insitute (JASRI), SPring-8, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo, 679-5198 Japan

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Prof. Yoshiki Kubota

Prof. Yoshiki Kubota

Department of Physical Science, Graduate School of Science, Osaka Prefecture University, Sakai, Osaka, 599-8531 Japan

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Prof. Hirokazu Kobayashi

Corresponding Author

Prof. Hirokazu Kobayashi

Division of Chemistry, Graduate School of Science, Kyoto University, Kitashirakawa-Oiwakecho, Sakyo-ku, Kyoto 606–8502 Japan

PRESTO (Japan) Science and Technology Agency (JST), 4-1-8 Honcho, Kawaguchi, Saitama, 332-0012 Japan

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First published: 11 August 2021
Citations: 4

Abstract

We report on Cu/amUiO-66, a composite made of Cu nanoparticles (NPs) and amorphous [Zr6O4(OH)4(BDC)6] (amUiO-66, BDC=1,4-benzenedicarboxylate), and Cu-ZnO/amUiO-66 made of Cu-ZnO nanocomposites and amUiO-66. Both structures were obtained via a spray-drying method and characterized using high-resolution transmission electron microscopy, energy dispersive spectra, powder X-ray diffraction and extended X-ray absorption fine structure. The catalytic activity of Cu/amUiO-66 for CO2 hydrogenation to methanol was 3-fold that of Cu/crystalline UiO-66. Moreover, Cu-ZnO/amUiO-66 enhanced the methanol production rate by 1.5-fold compared with Cu/amUiO-66 and 2.5-fold compared with γ-Al2O3-supported Cu-ZnO nanocomposites (Cu-ZnO/γ-Al2O3) as the representative hydrogenation catalyst. The high catalytic performance was investigated using in situ Fourier transform IR spectra. This is a first report of a catalyst comprising metal NPs and an amorphous metal–organic framework in a gas-phase reaction.

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