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; Naoki Ogiwara; Megumi Mukoyoshi; Hiroshi Kitagawa; Tomokazu Yamamoto; Takaaki Toriyama; Syo Matsumura; Masaaki Haneda; Shogo Kawaguchi; Yoshiki Kubota; Hirokazu Kobayashi

doi:10.1002/anie.202110585

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, Naoki Ogiwara, Megumi Mukoyoshi, Hiroshi Kitagawa, Tomokazu Yamamoto, Takaaki Toriyama, Syo Matsumura, Masaaki Haneda, Shogo Kawaguchi, Yoshiki Kubota, Hirokazu Kobayashi

研究成果: ジャーナルへの寄稿 › 学術誌 › 査読

22 被引用数 (Scopus)

抄録

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.

本文言語	英語
ページ（範囲）	22283-22288
ページ数	6
ジャーナル	Angewandte Chemie - International Edition
巻	60
号	41
DOI	https://doi.org/10.1002/anie.202110585
出版ステータス	出版済み - 10月 4 2021

!!!All Science Journal Classification (ASJC) codes

触媒
化学 (全般)

文献へのアクセス

10.1002/anie.202110585

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「Fabrication of Integrated Copper-Based Nanoparticles/Amorphous Metal–Organic Framework by a Facile Spray-Drying Method: Highly Enhanced CO₂ Hydrogenation Activity for Methanol Synthesis」の研究トピックを掘り下げます。これらがまとまってユニークなフィンガープリントを構成します。

引用スタイル

Mitsuka, Y., Ogiwara, N., Mukoyoshi, M., Kitagawa, H., Yamamoto, T., Toriyama, T., Matsumura, S., Haneda, M., Kawaguchi, S., Kubota, Y., & Kobayashi, H. (2021). Fabrication of Integrated Copper-Based Nanoparticles/Amorphous Metal–Organic Framework by a Facile Spray-Drying Method: Highly Enhanced CO₂ Hydrogenation Activity for Methanol Synthesis. Angewandte Chemie - International Edition, 60(41), 22283-22288. https://doi.org/10.1002/anie.202110585

Fabrication of Integrated Copper-Based Nanoparticles/Amorphous Metal–Organic Framework by a Facile Spray-Drying Method: Highly Enhanced CO₂ Hydrogenation Activity for Methanol Synthesis. / Mitsuka, Yuko; Ogiwara, Naoki; Mukoyoshi, Megumi その他.
In: Angewandte Chemie - International Edition, Vol. 60, No. 41, 04.10.2021, p. 22283-22288.

研究成果: ジャーナルへの寄稿 › 学術誌 › 査読

Mitsuka, Y, Ogiwara, N, Mukoyoshi, M, Kitagawa, H, Yamamoto, T , Toriyama, T, Matsumura, S, Haneda, M, Kawaguchi, S, Kubota, Y & Kobayashi, H 2021, 'Fabrication of Integrated Copper-Based Nanoparticles/Amorphous Metal–Organic Framework by a Facile Spray-Drying Method: Highly Enhanced CO₂ Hydrogenation Activity for Methanol Synthesis', Angewandte Chemie - International Edition, vol. 60, no. 41, pp. 22283-22288. https://doi.org/10.1002/anie.202110585

Mitsuka Y, Ogiwara N, Mukoyoshi M, Kitagawa H, Yamamoto T , Toriyama T その他. Fabrication of Integrated Copper-Based Nanoparticles/Amorphous Metal–Organic Framework by a Facile Spray-Drying Method: Highly Enhanced CO₂ Hydrogenation Activity for Methanol Synthesis. Angewandte Chemie - International Edition. 2021 10月 4;60(41):22283-22288. doi: 10.1002/anie.202110585

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

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.",

author = "Yuko Mitsuka and Naoki Ogiwara and Megumi Mukoyoshi and Hiroshi Kitagawa and Tomokazu Yamamoto and Takaaki Toriyama and Syo Matsumura and Masaaki Haneda and Shogo Kawaguchi and Yoshiki Kubota and Hirokazu Kobayashi",

note = "Funding Information: This work was supported by NEDO, JST PRESTO (No. JPMJPR1514) and a Grant‐in‐Aid for Scientific Research (B) (No. 17750056) from JSPS. The synchrotron radiation experiments were performed at the BL02B2 and BL14B2 lines of SPring‐8 with the approval of JASRI (Proposal No. 2018B1501, 2018B1728, 2019A1232 and 2019B1468). We are thankful to Dr. T. Honma of JASRI for technical support during the collection of X‐ray adsorption spectra. The STEM observations were partly supported by the Advanced Characterization Platform of the Nanotechnology Platform Japan (JPMXP09‐A‐19‐KU‐0292) sponsored by the Ministry of Education, Culture, Sports, Science and Technology of Japan. Funding Information: This work was supported by NEDO, JST PRESTO (No. JPMJPR1514) and a Grant-in-Aid for Scientific Research (B) (No. 17750056) from JSPS. The synchrotron radiation experiments were performed at the BL02B2 and BL14B2 lines of SPring-8 with the approval of JASRI (Proposal No. 2018B1501, 2018B1728, 2019A1232 and 2019B1468). We are thankful to Dr. T. Honma of JASRI for technical support during the collection of X-ray adsorption spectra. The STEM observations were partly supported by the Advanced Characterization Platform of the Nanotechnology Platform Japan (JPMXP09-A-19-KU-0292) sponsored by the Ministry of Education, Culture, Sports, Science and Technology of Japan. Publisher Copyright: {\textcopyright} 2021 Wiley-VCH GmbH",

year = "2021",

month = oct,

day = "4",

doi = "10.1002/anie.202110585",

language = "English",

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T1 - Fabrication of Integrated Copper-Based Nanoparticles/Amorphous Metal–Organic Framework by a Facile Spray-Drying Method

T2 - Highly Enhanced CO2 Hydrogenation Activity for Methanol Synthesis

AU - Mitsuka, Yuko

AU - Ogiwara, Naoki

AU - Mukoyoshi, Megumi

AU - Kitagawa, Hiroshi

AU - Yamamoto, Tomokazu

AU - Toriyama, Takaaki

AU - Matsumura, Syo

AU - Haneda, Masaaki

AU - Kawaguchi, Shogo

AU - Kubota, Yoshiki

AU - Kobayashi, Hirokazu

N1 - Funding Information: This work was supported by NEDO, JST PRESTO (No. JPMJPR1514) and a Grant‐in‐Aid for Scientific Research (B) (No. 17750056) from JSPS. The synchrotron radiation experiments were performed at the BL02B2 and BL14B2 lines of SPring‐8 with the approval of JASRI (Proposal No. 2018B1501, 2018B1728, 2019A1232 and 2019B1468). We are thankful to Dr. T. Honma of JASRI for technical support during the collection of X‐ray adsorption spectra. The STEM observations were partly supported by the Advanced Characterization Platform of the Nanotechnology Platform Japan (JPMXP09‐A‐19‐KU‐0292) sponsored by the Ministry of Education, Culture, Sports, Science and Technology of Japan. Funding Information: This work was supported by NEDO, JST PRESTO (No. JPMJPR1514) and a Grant-in-Aid for Scientific Research (B) (No. 17750056) from JSPS. The synchrotron radiation experiments were performed at the BL02B2 and BL14B2 lines of SPring-8 with the approval of JASRI (Proposal No. 2018B1501, 2018B1728, 2019A1232 and 2019B1468). We are thankful to Dr. T. Honma of JASRI for technical support during the collection of X-ray adsorption spectra. The STEM observations were partly supported by the Advanced Characterization Platform of the Nanotechnology Platform Japan (JPMXP09-A-19-KU-0292) sponsored by the Ministry of Education, Culture, Sports, Science and Technology of Japan. Publisher Copyright: © 2021 Wiley-VCH GmbH

PY - 2021/10/4

Y1 - 2021/10/4

N2 - 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.

AB - 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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