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Development of a new size-control method for nano-crystalline zeolite and its rational design as a catalyst

Research Project

Project/Area Number 22560755
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Reaction engineering/Process system
Research InstitutionHokkaido University

Principal Investigator

TAGO Teruoki  北海道大学, 大学院・工学研究院, 准教授 (20304743)

Co-Investigator(Kenkyū-buntansha) MASUDA Takao  北海道大学, 大学院・工学研究院, 教授 (20165715)
NAKASAKA Yuta  北海道大学, 大学院・工学研究院, 助教 (30629548)
Project Period (FY) 2010 – 2012
Project Status Completed (Fiscal Year 2012)
Budget Amount *help
¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000)
Fiscal Year 2012: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
Fiscal Year 2011: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2010: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Keywords反応速度 / 化学工学 / 触媒・化学プロセス / ナノゼオライト / 触媒設計 / アルキル化 / 脱水反応 / ナノ結晶ゼオライト / 構造規定剤フリー合成 / 界面活性剤添加効果 / 酸点不活性化 / 有機シラン化合物 / 芳香族アルキル化 / アルコール脱水反応
Research Abstract

Main objective of this research is a size-controlled synthesis for zeolite crystal and a development of design method for nano-zeolite catalyst. Various types of zeolites (MFI, TON, MOR, BEA, FAU and MTW) were synthesized and their crystal sizes could be successfully controlled. Especially, in MFI-,MOR-,MTW-,TON-type zeolites, the nano-crystalline zeolites with the size below 100 nm and macro-crystalline zeolite with the size above 1000 nm were obtained.Acrolein production from glycerol and 2,6-dimethyl naphthalene (2,6-DMN) production from 2-methyl naphthalene were conducted using zeolite catalysts. It is found that TON zeolite exhibits a high yield of acrolein above 80 % and that 2,6-DMN is selectively produced using MFI and MTW zeolites. Moreover, the crystal sizes of zeolite affect the product selectivity as well as the catalyst stability, the values of which are drastically improved by applying the nano-crystalline zeolite as a catalyst.

Report

(4 results)
  • 2012 Annual Research Report   Final Research Report ( PDF )
  • 2011 Annual Research Report
  • 2010 Annual Research Report
  • Research Products

    (53 results)

All 2013 2012 2011 2010 Other

All Journal Article (9 results) (of which Peer Reviewed: 9 results) Presentation (39 results) (of which Invited: 3 results) Book (4 results) Remarks (1 results)

  • [Journal Article] Effectiveness of Nano-scale ZSM-5 Zeolite and its Deactivation Mechanism on Catalytic Cracking of Representative Hydrocarbons of Naphtha2013

    • Author(s)
      H. Konno
    • Journal Title

      Microporous and Mesoporous Materials

      Volume: 175 Pages: 25-33

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis of nano-sized zeolites and their applications to zeolite membranes2012

    • Author(s)
      T. Tago, Y. Nakasaka and T. Masuda
    • Journal Title

      J. Jpn Petrol. Instit

      Pages: 149-159

    • Related Report
      2012 Final Research Report
    • Peer Reviewed
  • [Journal Article] Size-controlled synthesis of nano-zeolites and their application to light olefin synthesis2012

    • Author(s)
      T. Tago, H. Konno, Y. Nakasaka, T. Masuda
    • Journal Title

      Catal. Surv. fromAsia

      Volume: 16 Issue: 3 Pages: 148-163

    • DOI

      10.1007/s10563-012-9141-4

    • NAID

      120005323591

    • Related Report
      2012 Annual Research Report 2012 Final Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis of nano-sized zeolites and their applications to zeolite membranes2012

    • Author(s)
      T. Tago
    • Journal Title

      Journal of the Japan Petroleum Institute

      Volume: 55 Pages: 149-159

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Effects of crystal size and Si/Al ratio of MFI-type zeolite catalyst on light olefin synthesis by n-hexane cracking2012

    • Author(s)
      H. Konno
    • Journal Title

      Journal of the Japan Petroleum Institute

      Volume: 55 Pages: 267-274

    • DOI

      10.1016/j.cej.2012.06.157

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Kinetic Study for Burning Regeneration of Coked MFI-type Zeolite and Numerical Modeling for Regeneration Process in a Fixed-bed Reactor2012

    • Author(s)
      Y. Nakasaka
    • Journal Title

      Chemical Engineering Journal

      Volume: 207-208 Pages: 368-376

    • DOI

      10.1016/j.cej.2012.06.138

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Selective synthesis for light olefins from acetone over ZSM-5 zeolites with nano- and macro-crystal sizes 403(1-2), 183-1912011

    • Author(s)
      T.Tago, H.Konno, M.Sakamoto, Y, Nakasaka, T.Masuda
    • Journal Title

      Applied Catalysis A : General

      Volume: 403(1-2) Issue: 1-2 Pages: 183-191

    • DOI

      10.1016/j.apcata.2011.06.029

    • Related Report
      2012 Final Research Report 2011 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Preparation of Nano-Crystalline MFI Zeolite via Hydrothermal Synthesis in Water/Surfactant/Organic Solvent using Fumed Silica as the Si Source2011

    • Author(s)
      K.Iwakai, T.Tago, H.Konno, Y.Nakasaka, T.Masuda
    • Journal Title

      Microporous and Mesoporous Materials

      Volume: 141(1-3) Issue: 1-3 Pages: 167-174

    • DOI

      10.1016/j.micromeso.2010.11.001

    • NAID

      120002989226

    • Related Report
      2011 Annual Research Report 2010 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Selective production of isobutylene from acetone over alkali metal ion-exchanged BEA zeolites2011

    • Author(s)
      T.Tago, H.Konno, S.Ikeda, W.Ninomiya, S.Yamazaki, Y.Nakasaka, T.Masuda
    • Journal Title

      Catalysis Today

      Volume: 164(1) Issue: 1 Pages: 158-162

    • DOI

      10.1016/j.cattod.2010.10.034

    • Related Report
      2011 Annual Research Report 2010 Annual Research Report
    • Peer Reviewed
  • [Presentation] 炭素資源転換における触媒技術の動向と展望2013

    • Author(s)
      多湖輝興
    • Organizer
      石炭・炭素資源利用技術第148委員会 第138回研究会
    • Place of Presentation
      北海道大学 (札幌市)
    • Related Report
      2012 Annual Research Report
    • Invited
  • [Presentation] Isobutylene synthesis from water-containing acetone over potassium-exchanged BEA zeolite2013

    • Author(s)
      T. Tago
    • Organizer
      3rd North American Symposium on Chemical Reaction Engineering
    • Place of Presentation
      Westin Galleria Houston (USA)
    • Related Report
      2012 Annual Research Report
  • [Presentation] Size/morphology controlled synthesis of zeolite crystals and their applications2012

    • Author(s)
      T. Tago
    • Organizer
      10th Japan-Korea Symposium on Materials and Interfaces
    • Place of Presentation
      Coop Inn Kyoto, Japan
    • Year and Date
      2012-11-07
    • Related Report
      2012 Final Research Report
  • [Presentation] Catalytic Cracking of n-Hexane Cracking over MFI-Type Zeolites with Different Crystal Sizes2012

    • Author(s)
      T. Tago
    • Organizer
      22th International Symposium on Chemical Reaction Engineering
    • Place of Presentation
      the Maastricht Exhibition & Congress Centers, The Netherlands
    • Year and Date
      2012-09-04
    • Related Report
      2012 Final Research Report
  • [Presentation] Production of Light Olefins from n-Hexane Cracking over MFI Zeolites with Nano- and Macro-Crystal Sizes2012

    • Author(s)
      T. Tago
    • Organizer
      The 15th International Congress on Catalysis
    • Place of Presentation
      Messe Munchen (Germany)
    • Related Report
      2012 Annual Research Report
  • [Presentation] Selective production of isobutylene from water-containing acetone over BEA zeolite2012

    • Author(s)
      T. Tago
    • Organizer
      International Symposium on Zeolites and MicroPorous Crystals
    • Place of Presentation
      アステールプラザ (広島市)
    • Related Report
      2012 Annual Research Report
  • [Presentation] Kinetc Analysis of Burning Regeneration of Coked MFI-type Zeolites Obtained by Catalytic Cracking of n-Hexane2012

    • Author(s)
      T. Tago
    • Organizer
      22th International Symposium on Chemical Reaction Engineering
    • Place of Presentation
      MECC Maastricht (The Netherlands)
    • Related Report
      2012 Annual Research Report
  • [Presentation] Size/morphology controlled synthesis of zeolite crystals and their applications2012

    • Author(s)
      T. Tago
    • Organizer
      10th Japan-Korea Symposium on Materials and Interfaces
    • Place of Presentation
      コープイン京都 (京都市)
    • Related Report
      2012 Annual Research Report
    • Invited
  • [Presentation] ナノゼオライト積層触媒膜によるレフィン合成2012

    • Author(s)
      多湖輝興
    • Organizer
      化学工会反応工学部会 反応分離科会「反応分離シンポジウム 2012
    • Place of Presentation
      産総研つくば中央 (つくば市)
    • Related Report
      2012 Annual Research Report
    • Invited
  • [Presentation] Novel Synthesis for Zeolite Nanocrystals and Their Applications2011

    • Author(s)
      T.Tago, T.Masuda
    • Organizer
      14th Asian Chemical Congress 2011
    • Place of Presentation
      Queen Sirikit National Convention Centre, Bangkok(Thailand)(invited lecture)
    • Year and Date
      2011-09-07
    • Related Report
      2011 Annual Research Report
  • [Presentation] Selective Production of Intermediate Species of Reaction in Series Using Catalytic Zeolite Membrane as Contactor2011

    • Author(s)
      T.Masuda, T.Tago
    • Organizer
      The 12th Kuwait/Japan Joint Symposium
    • Place of Presentation
      Kuwait, Al Ahmadi, Kuwait Institute for Scientific Research (KISR) 招待講演
    • Related Report
      2010 Annual Research Report
  • [Presentation] 結晶サイズの異なるZSM-5ゼオライトを用いたn-ヘキサン接触分解による低級オレフィン選択合成2011

    • Author(s)
      今野大輝, 岡村拓哉, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      化学系学協会北海道支部2011年冬季研究発表会
    • Place of Presentation
      札幌,北海道大学学術交流会館
    • Related Report
      2010 Annual Research Report
  • [Presentation] MFI型ゼオライト細孔内におけるn-ヘキサンの気相拡散係数2011

    • Author(s)
      川原貴仁, 今野大輝, 岡村拓哉, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      化学系学協会北海道支部2011年冬季研究発表会
    • Place of Presentation
      札幌,北海道大学学術交流会館
    • Related Report
      2010 Annual Research Report
  • [Presentation] イオン交換ゼオライトによる亜酸化窒素の直接分解2011

    • Author(s)
      天池真輝, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第20回化学工学・紛体工学研究発表会
    • Place of Presentation
      札幌,JSTイノベーションプラザ北海道
    • Related Report
      2010 Annual Research Report
  • [Presentation] アセトンからの低級オレフィンの選択的合成を可能とするゼオライトナノクリスタル積層触媒膜の開発2011

    • Author(s)
      佐藤良多, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第20回化学工学・紛体工学研究発表会
    • Place of Presentation
      札幌,JSTイノベーションプラザ北海道
    • Related Report
      2010 Annual Research Report
  • [Presentation] ナノ結晶MFI型ゼオライトによるn-ヘキサンの接触分解2011

    • Author(s)
      今野大輝, 岡村拓哉, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第107回触媒討論会
    • Place of Presentation
      東京,首都大学東京
    • Related Report
      2010 Annual Research Report
  • [Presentation] MFI型ゼオライト触媒によるn-ヘキサン接触分解の速度解析2011

    • Author(s)
      岡村拓哉, 今野大輝, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第107回触媒討論会
    • Place of Presentation
      東京,首都大学東京
    • Related Report
      2010 Annual Research Report
  • [Presentation] ナノサイズMORゼオライトの構造規定剤フリー合成における界面活性添加効果2011

    • Author(s)
      藤原沙緒梨, 谷口太一, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第107回触媒討論会
    • Place of Presentation
      東京,首都大学東京
    • Related Report
      2010 Annual Research Report
  • [Presentation] Liquid phase Diffusivity of Benzene within Porous Materials in Cyclohexane and Iso-propanol Solution2010

    • Author(s)
      Y.Nakasaka, T.Tago, K.Yano, T.Masuda
    • Organizer
      FOA10 (10th International Conference on Fundamentals of Adsorption)
    • Place of Presentation
      淡路夢舞台国際会議場,淡路市
    • Related Report
      2010 Annual Research Report
  • [Presentation] Preparation of Mordenite Nanocrystal-layered Membrane for Selective Separation of Water by Pervaporation2010

    • Author(s)
      Y.Nakasaka, T.Tago, Y.Sato, R.Hashimoto, T.Masuda
    • Organizer
      5th International Zeolite Membrane Meeting
    • Place of Presentation
      Greece, Loutraki, Club Hotel Casino Loutrak
    • Related Report
      2010 Annual Research Report
  • [Presentation] Olefins Synthesis From Acetone Over Size-Controlled Zeolite Nanocrystals : Effect of Crystal Size on Catalitic Activity and Stability2010

    • Author(s)
      T.Tago, M.Sakamoto, H.Konno, Y.Nakasaka, T. Masuda
    • Organizer
      21st International Symposium on Chemical Reaction Engineering
    • Place of Presentation
      America, Philadelphia, Loews Philadelphia Hotel
    • Related Report
      2010 Annual Research Report
  • [Presentation] Synthetic Mechanism of Nano-Crystalline Zeolite in Water/Surfactant/Organic Solvent-Effect of Surfactant Concentration on Crystal Size-2010

    • Author(s)
      T.Tago, Y.Nakasaka, T.Masuda
    • Organizer
      16th International Zeolite Conference joint with the 7th International Mesostructured Materials Symposium
    • Place of Presentation
      Italy, Sorrento, Convention Center "Hilton Sorrento Palace"
    • Related Report
      2010 Annual Research Report
  • [Presentation] Measurement of Benzene Diffusivity within Porous Materials in Cyclohexane and Iso-propanol Solution2010

    • Author(s)
      Y.Nakasaka, T.Tago, K.Yano, T.Masuda
    • Organizer
      16th International Zeolite Conference joint with the 7th International Mesostructured Materials Symposium
    • Place of Presentation
      Italy, Sorrento, Convention Center "Hilton Sorrento Palace"
    • Related Report
      2010 Annual Research Report
  • [Presentation] Selective production of isobutylene from acetone over ion-exchanged BEA zeolites2010

    • Author(s)
      T.Tago, H.Konno, S.Ikeda, W.Ninomiya, Y.Nakasaka, T.Masuda
    • Organizer
      TOCAT6/APCAT5
    • Place of Presentation
      札幌,札幌コンベンションセンター
    • Related Report
      2010 Annual Research Report
  • [Presentation] Intracrystalline Diffusivity of Benzene within Micro-, Meso-porous Materials in Cyclohexane and Iso-propanol Solution2010

    • Author(s)
      Y.Nakasaka, T.Tago, K.Yano, T.Masuda
    • Organizer
      TOCAT6/APCAT5
    • Place of Presentation
      札幌,札幌コンベンションセンター
    • Related Report
      2010 Annual Research Report
  • [Presentation] 修飾Fe-ZSM-5ゼオライトを用いた形状選択的酸化反応2010

    • Author(s)
      佐藤陽平, 多湖輝興, 井上康信, 佐々木隆, 増田隆夫
    • Organizer
      触媒学会第50回オーロラセミナー
    • Place of Presentation
      洞爺湖町,トーヤ温泉ホテル
    • Related Report
      2010 Annual Research Report
  • [Presentation] ゼオライトナノクリスタル積層触媒膜によるアセトンからの低級オレフィンの選択的合成2010

    • Author(s)
      佐藤良多, 多湖輝興, 増田隆夫
    • Organizer
      触媒学会第50回オーロラセミナー
    • Place of Presentation
      洞爺湖町,トーヤ温泉ホテル
    • Related Report
      2010 Annual Research Report
  • [Presentation] イオン交換ゼオライト触媒による窒素酸化物の吸着・分解特性評価2010

    • Author(s)
      天池真輝, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      触媒学会第50回オーロラセミナー
    • Place of Presentation
      洞爺湖町,トーヤ温泉ホテル
    • Related Report
      2010 Annual Research Report
  • [Presentation] Silicalite-1細孔内におけるn-ヘキサンの吸着・拡散現象2010

    • Author(s)
      川原貴仁, 今野大輝, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      触媒学会第50回オーロラセミナー
    • Place of Presentation
      洞爺湖町,トーヤ温泉ホテル
    • Related Report
      2010 Annual Research Report
  • [Presentation] ナノサイズゼオライトの合成と応用-結晶サイズの影響-2010

    • Author(s)
      多湖輝興
    • Organizer
      触媒学会第50回オーロラセミナー
    • Place of Presentation
      洞爺湖町,トーヤ温泉ホテル 招待講演
    • Related Report
      2010 Annual Research Report
  • [Presentation] イオン交換ゼオライト触媒を用いたアセトンからのイソブテン選択合成2010

    • Author(s)
      山崎聖治, 今野大輝, 中坂佑太, 二宮航, 多湖輝興, 増田隆夫
    • Organizer
      化学工学会第42回秋季大会
    • Place of Presentation
      京都市,同志社大学今出川キャンパス
    • Related Report
      2010 Annual Research Report
  • [Presentation] ヘキサンクラッキングによる低級オレフィン選択的合成におけるMFI型ゼオライトの結晶サイズの影響2010

    • Author(s)
      今野大輝, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第106回触媒討論会
    • Place of Presentation
      甲府市,山梨大学甲府キャンパス
    • Related Report
      2010 Annual Research Report
  • [Presentation] 有機構造規定剤を使用しないナノ結晶MFIゼオライト合成における界面活性剤添加効果2010

    • Author(s)
      多湖輝興, 藤原沙緒梨, 今野大輝, 中坂佑太, 遠子内渉, 増田隆夫
    • Organizer
      第106回触媒討論会
    • Place of Presentation
      甲府市,山梨大学甲府キャンパス
    • Related Report
      2010 Annual Research Report
  • [Presentation] イオン交換ゼオライト触媒を用いた窒素酸化物の直接分解2010

    • Author(s)
      天池真輝, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第106回触媒討論会
    • Place of Presentation
      甲府市,山梨大学甲府キャンパス
    • Related Report
      2010 Annual Research Report
  • [Presentation] MFI型ゼオライト細孔内におけるn-ヘキサンの拡散係数測定2010

    • Author(s)
      川原貴仁, 今野大輝, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第106回触媒討論会
    • Place of Presentation
      甲府市,山梨大学甲府キャンパス
    • Related Report
      2010 Annual Research Report
  • [Presentation] ナノサイズZSM-5ゼオライト積層触媒膜によるアセトンからの低級オレフィンの選択的合成2010

    • Author(s)
      佐藤良多, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第26回ゼオライト研究発表会
    • Place of Presentation
      東京,タワーホール船堀
    • Related Report
      2010 Annual Research Report
  • [Presentation] 親水性ゼオライト膜を用いた浸透気化分離による高濃度有機溶液からの水の分離機構2010

    • Author(s)
      佐藤由貴, 橋本龍馬, 中坂佑太, 多湖輝興, 増田隆夫
    • Organizer
      第26回ゼオライト研究発表会
    • Place of Presentation
      東京,タワーホール船堀
    • Related Report
      2010 Annual Research Report
  • [Presentation] 金属イオン交換ゼオライトを基材とした形状選択的酸化反応場の構築2010

    • Author(s)
      佐藤陽平, 多湖輝興, 井上康信, 佐々木隆, 増田隆夫
    • Organizer
      第26回ゼオライト研究発表会
    • Place of Presentation
      東京,タワーホール船堀
    • Related Report
      2010 Annual Research Report
  • [Presentation] 水蒸気共存下におけるイオン交換ゼオライトを用いた窒素酸化物の直接分解2010

    • Author(s)
      中坂佑太, 天池真輝, 多湖輝興, 増田隆夫
    • Organizer
      第26回ゼオライト研究発表会
    • Place of Presentation
      東京,タワーホール船堀
    • Related Report
      2010 Annual Research Report
  • [Book] Zeolites: Synthesis, Chemistry and Applications, "Synthesis of nanocrystalline zeolites and their applications2012

    • Author(s)
      T. Tago, Y. Nakasaka and T. Masuda
    • Publisher
      NovaScientific publisher
    • Related Report
      2012 Final Research Report
  • [Book] Zeolites: Synthesis, Chemistry and Applications, Chapter 6 "Synthesis of nanocrystalline zeolites and their applications"2012

    • Author(s)
      T. Tago
    • Total Pages
      314
    • Publisher
      Nova Scientific publisher
    • Related Report
      2012 Annual Research Report
  • [Book] Zeolite Nanocrystals -Synthesis and Applications-2010

    • Author(s)
      T. Tago and T. Masuda, SCIYO, Nanocrystals
    • Related Report
      2012 Final Research Report
  • [Book] 『Nanocrystals』-Zeolite Nanocrystals-Synthesis and Applications-2010

    • Author(s)
      T.Tago, T.Masuda
    • Publisher
      SCIYO
    • Related Report
      2010 Annual Research Report
  • [Remarks]

    • URL

      http://cp1-ms.eng.hokudai.ac.jp/

    • Related Report
      2010 Annual Research Report

URL: 

Published: 2010-08-23   Modified: 2019-07-29  

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