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2015 Fiscal Year Annual Research Report

階層構造を持つミクロ-メソ多孔性複合材料の創成とその触媒機能の解明

Research Project

Project/Area Number 25289286
Research InstitutionMie University

Principal Investigator

石原 篤  三重大学, 工学(系)研究科(研究院), 教授 (60212908)

Co-Investigator(Kenkyū-buntansha) 橋本 忠範  三重大学, 工学(系)研究科(研究院), 准教授 (10271016)
那須 弘行  三重大学, 工学(系)研究科(研究院), 准教授 (20189179)
Project Period (FY) 2013-04-01 – 2016-03-31
Keywords階層構造触媒 / ゲル骨格補強法 / ゼオライト含有触媒 / 接触分解 / キュリーポイントパイロライザー法 / 減圧軽油 / 常圧残油 / 油脂
Outline of Annual Research Achievements

当研究室で開発したゲル骨格補強法大細孔径シリカと二層の階層構造を有するゼオライト含有シリカ-アルミナとを組み合わせることにより、新しいミクロ-メソ-メソの三層構造を有する触媒を調製し、その触媒反応特性を明らかにした。(成果1)三層構造のもっとも外側のシリカ層を作製するために、シリカ-ゲルの骨格補強をヘキサメチルジシロキサンと無水酢酸の組み合わせでトリメチルシリル化し、焼成後細孔容積5cm3/g、細孔径40nmに及ぶ大きな細孔を持つシリカを得ることができた。まず、この物質とゼオライトとの混合触媒によるn-ドデカンの接触分解において、細孔径が大きくなるにつれて活性および生成物選択性、特に分子生成物選択性が向上することが分かった。(成果2)成果1の細孔径の異なる触媒を用いて、CPP法により減圧軽油(VGO)と常圧残油(AR)の接触分解を検討した結果、VGOでは細孔径の影響が顕著であったが、ARでは細孔径の影響が極めて小さいことが分かった。これは、沸点範囲が反応温度よりも高い成分を半分以上含むARでは、触媒細孔中での拡散そのものが進行しなかった可能性が考えられる。(成果3)成果1によるゲル骨格補強シリカゲルを焼成前に、当研究室ですでに開発している2層構造触媒と混合することにより、3層構造触媒を調製した。窒素吸脱着測定の結果、吸着等温線に二つのヒステリシスが観察され、三層構造を形成していることが分かった。TEMでもゼオライトを含む2層のリング状の構造を三層目のシリカが取り囲んでいる様子が観察できた。これを用いた油脂の接触分解を検討した結果、ゼオライトを25%以上含む場合に原料の2層構造触媒よりも高活性が得られた。上記いずれも重要な成果が得られ、研究業績中2013年以降の成果は本研究による。

Research Progress Status

27年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

27年度が最終年度であるため、記入しない。

Causes of Carryover

27年度が最終年度であるため、記入しない。

Expenditure Plan for Carryover Budget

27年度が最終年度であるため、記入しない。

  • Research Products

    (29 results)

All 2016 2015

All Journal Article (12 results) (of which Peer Reviewed: 9 results,  Open Access: 5 results,  Acknowledgement Compliant: 5 results) Presentation (17 results) (of which Int'l Joint Research: 17 results)

  • [Journal Article] Catalytic cracking reaction of vacuum gas oil and atmospheric residue by zeolite-containing microporous andmesoporous composites using Curie point pyrolyzer2016

    • Author(s)
      Thanita Sonthisawate, Takehiro Nakanishi, Hiroyuki Nasu, Tadanori Hashimoto, Atsushi Ishihara
    • Journal Title

      Fuel Processing Technology

      Volume: 142 Pages: 337-344

    • DOI

      http://dx.doi.org/10.1016/j.fuproc.2015.10.016

    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Preparation of SiO2 and SiO2-Al2O3 catalysts by gel skeletal reinforcement using hexamethyldisiloxane and acetic anhydride system and elucidation of their catalytic cracking properties as matrices2016

    • Author(s)
      Atsushi Ishihara, Hiroaki Oono, Tadanori Hashimoto and Hiroyuki Nasu
    • Journal Title

      Microporous and Mesoporous Materials

      Volume: 230 Pages: 印刷中

    • DOI

      http://dx.doi.org/10.1016/j.micromeso.2016.01.025

    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Preparation and Photocatalytic Activity of Porous Bi2O3 polymorphism2016

    • Author(s)
      Tadanori Hashimoto, Honami Ohta, Hiroyuki Nasu and Atsushi Ishihara
    • Journal Title

      International Journal of Hydrogen Energy

      Volume: 41 Pages: 印刷中

    • DOI

      http://dx.doi.org/10.1016/j.ijhydene.2016.03.109

    • Peer Reviewed
  • [Journal Article] Catalytic cracking reaction of soybean oil by zeolite-containing microporous and mesoporous mixed catalysts using Curie point pyrolyzer2016

    • Author(s)
      Thanita Sonthisawate, Hiroyuki Nasu, Tadanori Hashimoto and Atsushi Ishihara
    • Journal Title

      Journal of the Japan Petroleum Institute

      Volume: 59 Pages: 印刷中

    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] 時評[「認定トライみたいなもの」2016

    • Author(s)
      石原 篤
    • Journal Title

      ペトロテック

      Volume: 39 Pages: 83-83

    • Open Access
  • [Journal Article] Hydrothermal gasification of phenol water on novel carbon-supported Ni catalysts prepared by the sol-gel method using tartaric acid and alminum tri-sec-butoxide2015

    • Author(s)
      Atsushi Ishihara, Tatsuya Imai, Tadanori Hashimoto, Hiroyuki Nasu
    • Journal Title

      Fuel Processing Technology

      Volume: 136 Pages: 34-40

    • DOI

      http://dx.doi.org/10.1016/j.fuproc.2014.07.040

    • Peer Reviewed
  • [Journal Article] Catalytic Cracking of VGO by Zeolite-Kaolin Mixed Catalysts Using Curie Point Pyrolyzer2015

    • Author(s)
      Atsushi Ishihara, Kentarou Kimura, Tadanori Hashimoto, Hiroyuki Nasu
    • Journal Title

      Journal of the Japan Petroleum Institute

      Volume: 58 Pages: 169-175

    • DOI

      dx.doi.org/10.1627/jpi.58.169

    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] Effects of Types of Metal Oxides on Hydrothermal Gasification of Phenol over Novel Metal Oxide-Carbon Composite Supported Ni Catalysts Prepared by Sol-Gel Method2015

    • Author(s)
      Atsushi Ishihara, Kenta Imanishi, Tadanori Hashimoto, Hiroyuki Nasu
    • Journal Title

      Journal of the Japan Petroleum Institute

      Volume: 58 Pages: 302-311

    • DOI

      dx.doi.org/10.1627/jpi.58.302

    • Peer Reviewed / Open Access
  • [Journal Article] Drastic Dependence of the pH Sensitivity of Fe2O3-Bi2O3-B2O3 Hydrophobic Glasses with Composition2015

    • Author(s)
      Tadanori Hashimoto, Fumiya Murayama, Masashi Nakao, Hiroyuki Nasu, Atsushi Ishihara, Yuji Nishio
    • Journal Title

      Materials

      Volume: 8 Pages: 8624-8629

    • DOI

      doi:10.3390/ma8125480

    • Peer Reviewed / Open Access
  • [Journal Article] Preparation and properties of sol-gel derived CuFeO2 thin films by dip-coating technique2015

    • Author(s)
      Hiroyuki Nasu、Masayuki Hasegawa, Tadanori Hashimoto Atsushi Ishihara, Koji Fujita and Katsuhisa Tanaka
    • Journal Title

      J. Ceram. Soc. Jpn.

      Volume: 123 Pages: 448-451

    • Peer Reviewed
  • [Journal Article] 接触分解触媒のための新しいメソ孔材料の調製とそれらの重質炭素資源接触分解反応特性2015

    • Author(s)
      石原 篤
    • Journal Title

      触媒

      Volume: 57 Pages: 87-93

    • Acknowledgement Compliant
  • [Journal Article] 時評「スマホがほしい」2015

    • Author(s)
      石原 篤
    • Journal Title

      触媒

      Volume: 57 Pages: 189-189

  • [Presentation] Selective dehydrocyclization of n-heptane using zeolite-alumina composite supported NiMo catalysts2015

    • Author(s)
      Atsushi Ishihara, Akihiro Itoh, Hiroyuki Nasu, Tadanori Hashimoto
    • Organizer
      Pacifichem 2015
    • Place of Presentation
      Hawaii, Honolulu, USA
    • Year and Date
      2015-12-15 – 2015-12-20
    • Int'l Joint Research
  • [Presentation] Estimation of catalytic cracking reaction of model compounds using zeolite-containing hierarchical silica and silica-alumina catalysts by Curie point pyrolyzer2015

    • Author(s)
      Atsushi Ishihara, Masashi Ninomiya, Hiroyuki Nasu, Tadanori Hashimoto
    • Organizer
      Pacifichem 2015
    • Place of Presentation
      Hawaii, Honolulu, USA
    • Year and Date
      2015-12-15 – 2015-12-20
    • Int'l Joint Research
  • [Presentation] Selective dehydrocyclization- cracking of soybean oil using zeolite-alumina composite supported PtNiMo catalysts2015

    • Author(s)
      Atsushi Ishihara, Takumi Ogiyama, Tadanori Hashimoto, Hiroyuki Nasu
    • Organizer
      Pacifichem 2015
    • Place of Presentation
      Hawaii, Honolulu, USA
    • Year and Date
      2015-12-15 – 2015-12-20
    • Int'l Joint Research
  • [Presentation] Catalytic cracking of heavy oil by hierarchical Y zeolite containing mesoporous silica-aluminas using Curie point pyrolyzer2015

    • Author(s)
      Thanita Sonthisawate, Takehiro Nakanishi, Tadanori Hashimoto, Hiroyuki Nasu, Atsushi Ishihara
    • Organizer
      The 5th International Symposium for Sustainability by Engineering at MIU (IS2 EMU 2015)
    • Place of Presentation
      三重大学 (三重県・津市)
    • Year and Date
      2015-09-29 – 2015-09-30
    • Int'l Joint Research
  • [Presentation] Hydrocracking of Atmospheric Residue by Zeolite-Alumina Containing Composite-Supported NiMo Catalysts Using Curie Point Pyrolyzer2015

    • Author(s)
      Syunya Ishida, Hiroyuki Nasu, Tadanori Hashimoto, Atsushi Ishihara
    • Organizer
      The 5th International Symposium for Sustainability by Engineering at MIU (IS2 EMU 2015)
    • Place of Presentation
      三重大学 (三重県・津市)
    • Year and Date
      2015-09-29 – 2015-09-30
    • Int'l Joint Research
  • [Presentation] Selective Dehydrocyclization of n-Heptane Using the Zeolite-Alumina Composite-Supported NiMo Catalysts2015

    • Author(s)
      Akihiro Itoh, Tadanori Hashimoto, Hiroyuki Nasu, Atsushi Ishihara
    • Organizer
      The 5th International Symposium for Sustainability by Engineering at MIU (IS2 EMU 2015)
    • Place of Presentation
      三重大学 (三重県・津市)
    • Year and Date
      2015-09-29 – 2015-09-30
    • Int'l Joint Research
  • [Presentation] Selective Dehydrocyclization-Cracking of Soybean Oil Using Zeolite-Alumina Composite Supported PtNiMo Catalysts2015

    • Author(s)
      Takumi Ogiyama, Hiroyuki Nasu, Tadanori Hashimoto, Atsushi Ishihara
    • Organizer
      The 5th International Symposium for Sustainability by Engineering at MIU (IS2 EMU 2015)
    • Place of Presentation
      三重大学 (三重県・津市)
    • Year and Date
      2015-09-29 – 2015-09-30
    • Int'l Joint Research
  • [Presentation] Analysis of Catalytic Cracking of C12-C32 Hydrocarbons by Hierarchical Zeolite-Containing Silica-Aluminas Using Curie Point Pyrolyzer2015

    • Author(s)
      Masashi Ninomiya , Hiroyuki Nasu, Tadanori Hashimoto, Atsushi Ishihara
    • Organizer
      The 5th International Symposium for Sustainability by Engineering at MIU (IS2 EMU 2015)
    • Place of Presentation
      三重大学 (三重県・津市)
    • Year and Date
      2015-09-29 – 2015-09-30
    • Int'l Joint Research
  • [Presentation] Preparation of Novel Carbon-Oxide Composite Supported Cobalt Catalysts and their Reactivity for Fischer-Tropsch Synthesis in the Presence of Solvent2015

    • Author(s)
      Yusuke Maejima, Hiroyuki Nasu, Tadanori Hashimoto, Atsushi Ishihara
    • Organizer
      The 5th International Symposium for Sustainability by Engineering at MIU (IS2 EMU 2015), September 29th 2015
    • Place of Presentation
      三重大学 (三重県・津市)
    • Year and Date
      2015-09-29 – 2015-09-30
    • Int'l Joint Research
  • [Presentation] Preparation and Photocatalytic Activity of TiO2-Bi2O32015

    • Author(s)
      Syunki Okada, Tadanori Hashimoto, Hiroyuki Nasu, Atsushi Ishihara
    • Organizer
      The 5th International Symposium for Sustainability by Engineering at MIU (IS2 EMU 2015)
    • Place of Presentation
      三重大学 (三重県・津市)
    • Year and Date
      2015-09-29 – 2015-09-30
    • Int'l Joint Research
  • [Presentation] Preparation of Novel Carbon-Oxide Composite Supported Cobalt Catalysts and Their Reactivity for Fischer-Tropsch Synthesis in the Presence of Solvent2015

    • Author(s)
      Atsushi Ishihara, Yusuke Maejima, Hiroyuki Nasu, Tadanori Hashimoto
    • Organizer
      The 13th China-Japan Coal and C1 Chemistry Symposium
    • Place of Presentation
      Dhunghang, China
    • Year and Date
      2015-08-31 – 2015-09-03
    • Int'l Joint Research
  • [Presentation] Elucidation of Catalytic Cracking of Soybean Oil by Zeolite-Mesoporous Oxides Composites Using Curie Point Pyrolyzer2015

    • Author(s)
      Atsushi Ishihara, Thanita Sonthisawate, Hiroyuki Nasu and Tadanori Hashimoto
    • Organizer
      The 13th China-Japan Coal and C1 Chemistry Symposium
    • Place of Presentation
      Dhunghang, China
    • Year and Date
      2015-08-31 – 2015-09-03
    • Int'l Joint Research
  • [Presentation] Catalytic Cracking of Soybean Oil by Different Hierarchical Zeolite Containing Mesoporous SiO2-Al2O3 Using a Curie Point Pyrolyzer2015

    • Author(s)
      Atsushi Ishihara, Daisuke Kawaraya, Thanita Sonthisawate, Hiroyuki Nasu, Tadanori Hashimoto
    • Organizer
      ACS, National Meeting, Div. Energy Fuels, Boston 2015
    • Place of Presentation
      Boston (USA)
    • Year and Date
      2015-08-16 – 2015-08-20
    • Int'l Joint Research
  • [Presentation] Catalytic Cracking of Heavy Oils by Hierarchical Zeolite Containing Mesoporous Silica-Aluminas with Large Mesopore Using Curie Point Pyrolyzer2015

    • Author(s)
      Atsushi Ishihara, Takehiro Nakanishi, Thanita Sonthisawate, Tadanori Hashimoto, Hiroyuki Nasu
    • Organizer
      ACS, National Meeting, Div. Energy Fuels, Boston 2015
    • Place of Presentation
      Boston (USA)
    • Year and Date
      2015-08-16 – 2015-08-20
    • Int'l Joint Research
  • [Presentation] Preparation and Photocatalytic Activity of Porous Bi2O32015

    • Author(s)
      Atsushi Ishihara, Tadanori Hashimoto, Honami Ohta, Hiroyuki Nasu
    • Organizer
      ACS, National Meeting, Div. Energy Fuels, Boston 2015
    • Place of Presentation
      Boston (USA)
    • Year and Date
      2015-08-16 – 2015-08-20
    • Int'l Joint Research
  • [Presentation] Catalytic cracking of soybean oil by three-layered hierarchical zeolite containing mesoporous SiO2-Al2O3 using a Curie point pyrolyzer2015

    • Author(s)
      Atsushi Ishihara, Daisuke Kawaraya, Thanita Sonthisawate, Tadanori Hashimoto, Hiroyuki Nasu
    • Organizer
      ZMPC2015
    • Place of Presentation
      札幌コンベンションセンター (北海道・札幌市)
    • Year and Date
      2015-06-28 – 2015-07-01
    • Int'l Joint Research
  • [Presentation] Preparation of SiO2 and SiO2-Al2O3 catalysts by gel skeletal reinforcement and analysis of catalytic cracking reaction of n-dodecane2015

    • Author(s)
      Atsushi Ishihara, Hiroaki Oono, Tadanori Hashimoto, Hiroyuki Nasu
    • Organizer
      ZMPC2015
    • Place of Presentation
      札幌コンベンションセンター (北海道・札幌市)
    • Year and Date
      2015-06-28 – 2015-07-01
    • Int'l Joint Research

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Published: 2017-01-06  

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