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Development of catalyst for one-stepoxidation of benzene with oxygen to phenol and improvement of its catalyst

Research Project

Project/Area Number 15K06566
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Research Field Catalyst/Resource chemical process
Research InstitutionKobe University

Principal Investigator

Ichihashi Yuichi  神戸大学, 工学研究科, 准教授 (20362759)

Co-Investigator(Kenkyū-buntansha) 西山 覚  神戸大学, 工学研究科, 教授 (00156126)
谷屋 啓太  神戸大学, 先端融合研究環, 助教 (30632822)
Co-Investigator(Renkei-kenkyūsha) TANIYA Keita  神戸大学, 先端融合研究環, 助教 (30632822)
Project Period (FY) 2015-04-01 – 2018-03-31
Project Status Completed (Fiscal Year 2017)
Budget Amount *help
¥4,940,000 (Direct Cost: ¥3,800,000、Indirect Cost: ¥1,140,000)
Fiscal Year 2017: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
Fiscal Year 2016: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2015: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000)
Keywords触媒反応 / 選択酸化 / フェノール合成 / Cu/HZSM-5 / DFT計算 / FT-IR / ベンゼンの気相接触酸化反応 / フェノール合成反応 / 銅担持ゼオライト触媒 / 量子化学計算 / 成形体触媒 / ルイス酸点 / 骨格外アルミ
Outline of Final Research Achievements

The gas-phase catalytic oxidation of benzene over copper supported on HZSM-5 added with Al (Cu/Al/HZSM-5) was carried out by using molecular oxygen as an oxidant. Phenol was effectively produced by Al addition to Cu/HZSM-5. It was also found that these catalysts calcined at higher temperature promoted the phenol formation for the benzene oxidation. FT-IR measurements of Cu/HZSM-5 catalysts indicated that the calcination of catalysts at higher temperature led to the formation of extra-framework Al species from zeolite framework and these extra-framework Al functioned as Lewis acid sites. And also, the aluminum addition to Cu/HZSM-5 catalysts caused the increase of extra-framework Al species and led to the increase of these Lewis acid sites. In this work, the detail mechanism of benzene oxidation over Cu/HZSM-5 catalysts was clarified by FT-IR measurements and DFT calculation. Moreover, it became successful to develop the molded Cu/HZSM-5 catalysts as industrial catalysts.

Report

(4 results)
  • 2017 Annual Research Report   Final Research Report ( PDF )
  • 2016 Research-status Report
  • 2015 Research-status Report
  • Research Products

    (20 results)

All 2017 2016 2015

All Journal Article (3 results) (of which Peer Reviewed: 3 results) Presentation (17 results) (of which Int'l Joint Research: 6 results,  Invited: 1 results)

  • [Journal Article] Direct oxidation of benzene with molecular oxygen in liquid phase catalysed by heterogeneous copper complexes encapsulated in Y-type zeolite2017

    • Author(s)
      A. Okemoto, K. Ueyama, K. Taniya, Y. Ichihashi, S. Nishiyama
    • Journal Title

      Catalysis Communications

      Volume: 100 Pages: 29-32

    • DOI

      10.1016/j.catcom.2017.06.013

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Selective catalytic oxidation of benzene over Cu/Ti/HZSM-5 under low oxygen pressure for one step synthesis of phenol2016

    • Author(s)
      Atushi Okemoto, Yo-hei Tsukano, Arisa Utsunomiya, Keita Taniya, Yuichi Ichihashi, Satoru Nishiyama
    • Journal Title

      Journal of Molecular Catalysis A: Chemical

      Volume: 411 Pages: 372-376

    • DOI

      10.1016/j.molcata.2015.11.007

    • Related Report
      2015 Research-status Report
    • Peer Reviewed
  • [Journal Article] Study of Benzene Hydroxylation in Liquid Phase Using Mono- and Binuclear Copper Complex Catalysts2015

    • Author(s)
      A. Okemoto, K. Kato, K. Taniya, Y. Ichihashi, S. Nishiyama
    • Journal Title

      Chemistry Letters

      Volume: 44 Issue: 3 Pages: 384-386

    • DOI

      10.1246/cl.141147

    • NAID

      130004868391

    • Related Report
      2015 Research-status Report
    • Peer Reviewed
  • [Presentation] バナジウム錯体触媒を用いた分子状酸素によるベンゼンの液相水酸化反応の機構解明2017

    • Author(s)
      桶本 篤史, 宇都宮 有咲, 井上 賀貴, 谷屋 啓太, 市橋 祐一, 西山 覚
    • Organizer
      化学工学会 第82回
    • Place of Presentation
      芝浦工業大学(東京都・江東区)
    • Year and Date
      2017-03-06
    • Related Report
      2016 Research-status Report
  • [Presentation] Mechanism study of gas-phase oxidation of benzene to phenol over Cu/HZSM-5 catalysts2017

    • Author(s)
      Y. Ichihashi, S. Watanabe, R. Araki, Y. Tsukano, A. Okemoto, K. Taniya, S. Nishiyama
    • Organizer
      13th European Congress on Catalysis (EUROPACAT2017)
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] バナジウム錯体触媒を用いた分子状酸素によるベンゼンの液相水酸化反応の機構解明2017

    • Author(s)
      桶本篤史、宇都宮有咲、井上賀貴、谷屋啓太、市橋祐一、西山覚
    • Organizer
      化学工学会 第82回年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 銅担持HZSM-5を用いたベンゼンの気相接触反応とその反応機構解明2017

    • Author(s)
      荒木凜、宇都宮有咲、桶本篤史、谷屋啓太、市橋祐一、西山覚
    • Organizer
      第19回化学工学会学生発表会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 銅担持HZSM-5を用いたベンゼンの気相接触反応とその反応機構解明2017

    • Author(s)
      荒木 凜, 宇都宮 有咲, 桶本 篤史, 谷屋 啓太, 市橋 祐一, 西山 覚
    • Organizer
      第19回化学工学会学生発表会
    • Place of Presentation
      大阪大学(大阪府・豊中市)
    • Related Report
      2016 Research-status Report
  • [Presentation] 銅二核錯体触媒を用いたベンゼンの液相酸化反応によるヒドロキノン一段階合成2016

    • Author(s)
      上山 耕平, 桶本 篤史, 谷屋 啓太, 市橋 祐一, 西山 覚
    • Organizer
      第46回石油・石油化学討論会
    • Place of Presentation
      京都リサーチパーク(京都府・京都市)
    • Year and Date
      2016-11-17
    • Related Report
      2016 Research-status Report
  • [Presentation] DFT計算を用いたバナジウム錯体触媒上でのベンゼンの液相酸化反応機構の解明2016

    • Author(s)
      宇都宮 有咲, 桶本 篤史, 谷屋 啓太, 市橋 祐一, 西山 覚
    • Organizer
      第49回酸化反応討論会
    • Place of Presentation
      徳島大学(徳島県・徳島市)
    • Year and Date
      2016-11-12
    • Related Report
      2016 Research-status Report
  • [Presentation] DFT計算を用いたバナジウム錯体触媒による酸素活性化過程の解析2016

    • Author(s)
      桶本 篤史, 宇都宮 有咲, 井上 賀貴, 谷屋 啓太, 市橋 祐一, 西山 覚
    • Organizer
      化学工学会 第48回秋季大会
    • Place of Presentation
      徳島大学(徳島県・徳島市)
    • Year and Date
      2016-09-06
    • Related Report
      2016 Research-status Report
  • [Presentation] Theoretical Study on Reaction Mechanism of Benzene Oxidation by Using Vanadium Complex Catalysts2016

    • Author(s)
      Atsushi Okemoto, Arisa Utsunomiya, Keita Taniya, Yuichi Ichihashi, Satoru Nishiyama
    • Organizer
      International Symposium on Nanostructured Photocatalysts and Catalysts
    • Place of Presentation
      Osaka University(Osaka・Suita)
    • Year and Date
      2016-04-08
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research
  • [Presentation] The Study of Reaction Mechanism for Benzene Oxidation over Cu/HZSM-5 Catalysts2016

    • Author(s)
      Yuichi Ichihashi, Atsushi Okemoto, Syun Watanabe, Keita Taniya, Satoru Nishiyama
    • Organizer
      International Symposium on Nanostructured Photocatalysts and Catalysts
    • Place of Presentation
      Osaka University(Osaka・Suita)
    • Year and Date
      2016-04-08
    • Related Report
      2016 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] The Study of Reaction Mechanism for Benzene Oxidation over Cu/HZSM-5 Catalysts2016

    • Author(s)
      Yuichi Ichihashi, Atsushi Okemoto, Syun Watanabe, Keita Taniya, Satoru Nishiyama
    • Organizer
      International Symposium on Nanostructured Photocatalysts and Catalysts (NPC2016)
    • Place of Presentation
      Osaka University (Osaka・Osaka)
    • Year and Date
      2016-04-08
    • Related Report
      2015 Research-status Report
    • Int'l Joint Research
  • [Presentation] 銅二核錯体を用いたベンゼンの液相酸化反応2016

    • Author(s)
      上山 耕平, 桶本 篤史, 谷屋 啓太, 市橋 祐一, 西山 覚
    • Organizer
      第9回触媒表面化学研究発表会
    • Place of Presentation
      関西大学(大阪府・吹田市)
    • Related Report
      2016 Research-status Report
  • [Presentation] 銅二核錯体触媒を用いたベンゼンの液相酸化反応2016

    • Author(s)
      上山 耕平, 桶本 篤史, 谷屋 啓太, 市橋 祐一, 西山 覚
    • Organizer
      第26回キャラクタライゼーション講習会
    • Place of Presentation
      大阪工業大学(大阪府・大阪市)
    • Related Report
      2016 Research-status Report
  • [Presentation] 銅ゼオライト触媒によるベンゼンの気相接触酸化反応へのTi添加効果2015

    • Author(s)
      橘政宏, 桶本篤史, 谷屋啓太, 市橋祐一, 西山覚
    • Organizer
      第48回酸化反応討論会
    • Place of Presentation
      同志社大学(京都府・京都市)
    • Year and Date
      2015-10-23
    • Related Report
      2015 Research-status Report
  • [Presentation] Study on Reaction Mechanism of Benzene Oxidation by Using Metal Complex Catalysts2015

    • Author(s)
      Atsushi Okemoto, Kurumi Kato, Arisa Utsunomiya, Keita Taniya, Yuichi Ichihashi, Satoru Nishiyama
    • Organizer
      Asian Pacific Confederation of Chemical Engineering (APCChE 2015)
    • Place of Presentation
      Melbourne, Australia
    • Year and Date
      2015-09-27
    • Related Report
      2015 Research-status Report
    • Int'l Joint Research
  • [Presentation] フェノール生成のための気相接触酸化反応におけるCu/HZSM-5へのTi添加効果2015

    • Author(s)
      橘政宏, 桶本篤史, 谷屋啓太, 市橋祐一, 西山覚
    • Organizer
      第116回触媒討論会
    • Place of Presentation
      三重大学 (三重県・津市)
    • Year and Date
      2015-09-16
    • Related Report
      2015 Research-status Report
  • [Presentation] Effect of Ti Addition to Cu/HZSM-5 Catalyst on Gas-Phase Oxidation of Benzene2015

    • Author(s)
      Masahiro Tachibana, Atsushi Okemoto, Keita Taniya, Yuichi Ichihashi, Satoru Nishiyama
    • Organizer
      International Symposium of Zeolite and Microporous Crystals 2015
    • Place of Presentation
      Sapporo Convention Center (Hokkaido・Sapporo)
    • Year and Date
      2015-06-28
    • Related Report
      2015 Research-status Report
    • Int'l Joint Research

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Published: 2015-04-16   Modified: 2019-03-29  

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