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2023 年度 実績報告書

触媒活性サイトの空間組織が反応に及ぼす影響研究

研究課題

研究課題/領域番号 22KJ1456
配分区分基金
研究機関富山大学

研究代表者

姚 杰  富山大学, 工学部, 特別研究員(PD)

研究期間 (年度) 2023-03-08 – 2024-03-31
キーワードZeolite / Dimethyl ether / Carbonylation
研究実績の概要

The design of heterogeneous catalysts traditionally centers on modifying their intrinsic physicochemical properties or adjusting electron states with additives at the sub-nanoscale level. However, constructing an entirely new reaction network, which entails a qualitative shift in reaction efficiency by disrupting the existing network, poses significant challenges.
In this research year, we utilized a reverse strategy: detaching one component (Cu) from its parent catalyst (MOR zeolite) on a centimeter scale to successfully reconstruct a completely new reaction network, achieving markedly improved catalytic performance of a record-breaking percentage gain of 266% in the space-time yield of methyl acetate product during the carbonylation of dimethyl ether.
In-situ high-pressure Synchrotron Vacuum Ultraviolet Photoionization Mass
Spectrometry, in-situ TEM, and in-situ DRIFTS were employed to make the brand-
new reaction mechanism clear. The previously unreported vital intermediate, acetic anhydride, was discovered for the first time when employing the detaching style of Cu/SiO2//H-MOR.
This noteworthy discovery not only underscores its profound implications but also emphasizes its extensive potential for deployment in designing various heterogeneous catalysts, applicable across a diverse array of chemical reactions.

  • 研究成果

    (6件)

すべて 2024 2023

すべて 雑誌論文 (4件) (うち国際共著 1件、 査読あり 4件、 オープンアクセス 1件) 学会発表 (2件) (うち国際学会 2件)

  • [雑誌論文] C1 Chemistry: The Stories of Research and Applications from Toyama2024

    • 著者名/発表者名
      Yao Jie、Cao Fenghai、Han Yu、Wang Yang、Tan Li、Sun Jian、Yang Guohui、Shi Lei
    • 雑誌名

      Resources Chemicals and Materials

      巻: 3 ページ: 62~92

    • DOI

      10.1016/j.recm.2023.08.004

    • 査読あり / オープンアクセス
  • [雑誌論文] Unveiling the Catalytic Role of Zeolite P1 in Carbonylation Reaction2024

    • 著者名/発表者名
      Fan Jiaqi、Yao Jie、Feng Xiaobo、Wang Chengwei、Shi Ying、Feng Haozhe、Gao Weizhe、He Yingluo、Guo Xiaoyu、Yasuda Shuhei、Yang Guohui、Tsubaki Noritatsu
    • 雑誌名

      Chem & Bio Engineering

      巻: 1 ページ: 141~149

    • DOI

      10.1021/cbe.3c00101

    • 査読あり
  • [雑誌論文] K-doped CuO/ZnO with dual active centers of synergism for highly efficient dimethyl carbonate synthesis2023

    • 著者名/発表者名
      Han Han, Xue Ye, Jie Yao, Xinhua Gao, Jinghao Yu, Lisheng Guo, Jie Li
    • 雑誌名

      AIChE JOURNAL

      巻: 69 ページ: e18158

    • DOI

      10.1002/aic.18158

    • 査読あり / 国際共著
  • [雑誌論文] Optimizing interfacial interaction between Cu and metal oxides boosts methanol yield in CO2 hydrogenation2023

    • 著者名/発表者名
      Li Xiaojun、Xia Yudong、Xu Yangzhou、Li Haitao、Huang Jiangchao、Yao Jie、Zhao Heng、Gao Xinhua、Yu Jinghao、Guo Lisheng、Li Jie
    • 雑誌名

      Research on Chemical Intermediates

      巻: 49 ページ: 3933~3950

    • DOI

      10.1007/s11164-023-05063-x

    • 査読あり
  • [学会発表] A Newfound Zeolite Catalyst for Highly Efficient Carbonylation2024

    • 著者名/発表者名
      Yao, J., Yang, G., Tsubaki, N.
    • 学会等名
      13th Natural Gas Conversion Symposium (NGCS13)
    • 国際学会
  • [学会発表] Ammonia Pools in Zeolites for Direct Fabrication of Catalytic Centers2023

    • 著者名/発表者名
      Yao, J., Yang, G., Tsubaki, N.
    • 学会等名
      InternationaConference on Clean and Efficient Utilization of Hydrocarbon Resources
    • 国際学会

URL: 

公開日: 2024-12-25  

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