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Mechanochemical Route for Preparation of MFI-Type Zeolites Containing Highly Dispersed and Small Ce Species and Catalytic Application to Low-Temperature Oxidative Coupling of Methane

  • Mizuho Yabushita*
    Mizuho Yabushita
    Department of Applied Chemistry, School of Engineering, Tohoku University, 6-6-07 Aoba, Aramaki, Aoba-ku, Sendai, Miyagi 980-8579, Japan
    *Email: [email protected]
  • Motohiro Yoshida
    Motohiro Yoshida
    Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
  • Ryota Osuga
    Ryota Osuga
    Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
    More by Ryota Osuga
  • Fumiya Muto
    Fumiya Muto
    Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
    More by Fumiya Muto
  • Shoji Iguchi
    Shoji Iguchi
    Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo 152-8552, Japan
    More by Shoji Iguchi
  • Shuhei Yasuda
    Shuhei Yasuda
    Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8503, Japan
  • Atsushi Neya
    Atsushi Neya
    Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
    More by Atsushi Neya
  • Mami Horie
    Mami Horie
    Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
    More by Mami Horie
  • Sachiko Maki
    Sachiko Maki
    Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
    International Center for Synchrotron Radiation Innovation Smart, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
    More by Sachiko Maki
  • Kiyoshi Kanie
    Kiyoshi Kanie
    Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
    International Center for Synchrotron Radiation Innovation Smart, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
  • Ichiro Yamanaka
    Ichiro Yamanaka
    Department of Chemical Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo 152-8552, Japan
    Core Research for Evolutional Science and Technology, Japan Science and Technology Agency, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan
  • Toshiyuki Yokoi
    Toshiyuki Yokoi
    Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama, Kanagawa 226-8503, Japan
  • , and 
  • Atsushi Muramatsu*
    Atsushi Muramatsu
    Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
    International Center for Synchrotron Radiation Innovation Smart, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan
    Core Research for Evolutional Science and Technology, Japan Science and Technology Agency, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan
    *Email: [email protected]
Cite this: Ind. Eng. Chem. Res. 2021, 60, 28, 10101–10111
Publication Date (Web):July 7, 2021
https://doi.org/10.1021/acs.iecr.1c01664
Copyright © 2021 American Chemical Society
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Abstract

MFI-type zeolites containing Ce species were prepared by a mechanochemically assisted two-step method, where first an amorphous Si–Ce–O composite was produced via a mechanochemical reaction of SiO2 and CeO2 and then transformed into an MFI-type zeolite under hydrothermal conditions. The Ce species in this sample were more highly dispersed than those in the two control materials: a Ce-containing MFI-type zeolite synthesized via the conventional one-pot hydrothermal approach and Ce species simply deposited on silicalite-1. The highly dispersed and small Ce species in the zeolite exhibited a unique catalytic performance for the oxidative conversion of methane after the impregnation of Pd species, and the combination of Pd and Ce species produced ethane even at reaction temperatures as low as 100–300 °C.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.iecr.1c01664.

  • STEM-EDS images of ball-milled mixtures, surface areas of synthesized MFI-type zeolites, NH3-TPD profiles for Ce-MFIMC and Ce-MFIHT, XRD patterns for 1 wt % M/Ce-MFIMC, comparison of catalytic performance of 1 wt % Pd/Ce-MFIMC and Na-Mn-W/SiO2, XRD patterns and reaction results for Pd/Ce-MFIMC with different Pd loadings, XRD patterns for 3 wt % Pd/support, H2-TPR profiles for Ce-MFIMC and 3 wt % Pd/Ce-MFIMC, and Pd K edge XAS spectra and STEM-EDS images of 3 wt % Pd/Ce-MFIMC (PDF)

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