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Creation of new-type zeolite catalysts and control of active sites that enable environmentally benign, highly efficient chemical processes

Research Project

Project/Area Number 15H04185
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Catalyst/Resource chemical process
Research InstitutionYokohama National University

Principal Investigator

Kubota Yoshihiro  横浜国立大学, 大学院工学研究院, 教授 (30283279)

Co-Investigator(Renkei-kenkyūsha) INAGAKI SATOSHI  横浜国立大学, 大学院工学研究院, 准教授 (90367037)
Project Period (FY) 2015-04-01 – 2018-03-31
Project Status Completed (Fiscal Year 2017)
Budget Amount *help
¥17,420,000 (Direct Cost: ¥13,400,000、Indirect Cost: ¥4,020,000)
Fiscal Year 2017: ¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2016: ¥5,850,000 (Direct Cost: ¥4,500,000、Indirect Cost: ¥1,350,000)
Fiscal Year 2015: ¥7,410,000 (Direct Cost: ¥5,700,000、Indirect Cost: ¥1,710,000)
Keywordsゼオライト合成 / ゼオライト触媒 / 固体酸 / DTO / 触媒活性点 / MCM-68 / YNU-5 / DTO反応 / 低級オレフィン / 希土類修飾 / 熱安定性 / 活性点制御 / 環境調和型プロセス / ジメチルエーテル / メタノール
Outline of Final Research Achievements

The acid characteristics of MCM-68 (Si/Al=10) and dealuminated MCM-68 with Si/Al of 35, 60 and 107 were evaluated using FT-IR spectroscopy. Collidine adsorbed only on the external acid sites at 303 K. A comparison of the CO stretching vibration frequencies confirmed that MCM-68(10) possessed two types of Lewis acid sites as well as Brønsted acid sites. Lewis acid sites originating from extra-framework aluminum species were readily removed. In the case of Lewis acid sites associated with Al species connected to Si atoms via shared O atoms, the slightly stronger acid sites were easily removed via dealumination.
As an unexpected achievement, we succeeded in the synthesizing a novel aluminosilicate zeolite YNU-5, the first zeolite containing interconnected 12-, 12- and 8-ring pores as well as independent straight 8-ring channels.

Report

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

    (37 results)

All 2017 2016 2015 Other

All Journal Article (9 results) (of which Peer Reviewed: 8 results,  Open Access: 1 results,  Acknowledgement Compliant: 4 results) Presentation (20 results) (of which Int'l Joint Research: 10 results,  Invited: 3 results) Book (2 results) Remarks (3 results) Patent(Industrial Property Rights) (2 results) (of which Overseas: 1 results) Funded Workshop (1 results)

  • [Journal Article] Selective Production of Light Olefins over MSE-type Zeolite Catalyst2017

    • Author(s)
      Q. Han, S. Park, S. Inagaki, Y. Kubota
    • Journal Title

      Journal of the Japan Petroleum Institute

      Volume: 60 Issue: 6 Pages: 288-300

    • DOI

      10.1627/jpi.60.288

    • NAID

      130006192166

    • ISSN
      1346-8804, 1349-273X
    • Year and Date
      2017-11-01
    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Catalytic performance of Ce-modified MCM-68 zeolite in the dimethyl ether-to-olefin reaction: Impact of high calcination temperature2017

    • Author(s)
      Q. Han, K. Enoeda, S. Inagaki, Y. Kubota
    • Journal Title

      Chemistry Letters

      Volume: 46 Issue: 9 Pages: 1434-1437

    • DOI

      10.1246/cl.170591

    • NAID

      130006067879

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] The microporous aluminosilicate with 12-, 12-, and 8-ring pores and isolated 8-ring channels2017

    • Author(s)
      N. Nakazawa, T. Ikeda (C.A.), H. Hiyoshi, Y. Yoshida, S. Inagaki and Y. Kubota
    • Journal Title

      J. Am. Chem. Soc.

      Volume: 139 Issue: 23 Pages: 7989-7997

    • DOI

      10.1021/jacs.7b03308

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Correction to “A microporous aluminosilicate with 12-, 12-, and 8-ring pores and isolated 8-ring channels"2017

    • Author(s)
      Naoto Nakazawa, Takuji Ikeda, Norihito Hiyoshi, , Yuka Yoshida, Qiao Han, Satoshi Inagaki, Yoshihiro Kubota
    • Journal Title

      J. Am. Chem. Soc.

      Volume: 139 Issue: 34 Pages: 12102-12102

    • DOI

      10.1021/jacs.7b08094

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 低級オレフィン製造用触媒としての新型ゼオライト2017

    • Author(s)
      窪田好浩,稲垣怜史,朴 成植
    • Journal Title

      工業材料

      Volume: 65 Pages: 23-28

    • Related Report
      2016 Annual Research Report
    • Acknowledgement Compliant
  • [Journal Article] Direct hydrothermal synthesis of high-silica SSZ-39 zeolite with small particle size2016

    • Author(s)
      N. Nakazawa, S. Inagaki, Y. Kubota
    • Journal Title

      Chemistry Letters

      Volume: 45 Issue: 8 Pages: 919-921

    • DOI

      10.1246/cl.160370

    • NAID

      130005254524

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Novel technique to synthesize AFX-type zeolite using a bulky and rigid diquaternary ammonium cation2016

    • Author(s)
      N. Nakazawa, S. Inagaki, Y. Kubota
    • Journal Title

      Advanced Porous Materials

      Volume: 4 Issue: 3 Pages: 219-229

    • DOI

      10.1166/apm.2016.1114

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Selective formation of light olefins from dimethyl ether over MCM-68 modified with phosphate species2016

    • Author(s)
      S. Park, S. Inagaki, Y. Kubota
    • Journal Title

      Catalysis Today

      Volume: 265 Pages: 218-224

    • DOI

      10.1016/j.cattod.2015.08.061

    • Related Report
      2016 Annual Research Report 2015 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] High-Performance Catalysts with MSE-Type Zeolite Framework2015

    • Author(s)
      Y. Kubota, S. Inagaki
    • Journal Title

      Topics in Catalysis

      Volume: 58 Issue: 7-9 Pages: 480-493

    • DOI

      10.1007/s11244-015-0389-6

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed
  • [Presentation] Synthetic investigation of AFX-type zeolite by using bulky and rigid diquaternary ammonium compound as organic structure-directing agent2017

    • Author(s)
      N. Nakazawa, S. Inagaki, Y. Kubota
    • Organizer
      3rd Euro-Asia Zeolite Conference
    • Place of Presentation
      Bali, Indonesia
    • Year and Date
      2017-01-22
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Seed-Directed Synthesis of MSE-type Zeolite using Simple Organic Structure-Directing Agent by Extending Composite Building Unit Hypothesis2017

    • Author(s)
      S. Sogukkanli, S.P. Elangovan, K. Itabashi, K. Iyoki, M. Takano, Z. Liu, S. Inagaki, T. Wakihara, Y. Kubota, T. Okubo
    • Organizer
      3rd Euro-Asia Zeolite Conference
    • Place of Presentation
      Bali, Indonesia
    • Year and Date
      2017-01-22
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 濃厚シリケート溶液から出発するゼオライトの水熱合成2017

    • Author(s)
      中澤直人,吉田友香,稲垣怜史,窪田好浩
    • Organizer
      第33回ゼオライト研究発表会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 希土類修飾を施したAl-MCM-68の固体酸触媒特性2017

    • Author(s)
      榎枝 築,韓 喬,稲垣怜史,窪田好浩
    • Organizer
      第33回ゼオライト研究発表会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 新規骨格ゼオライトYNU-5の固体酸触媒特性2017

    • Author(s)
      吉田友香,中澤直人,韓 喬,稲垣怜史,窪田好浩
    • Organizer
      第120回触媒討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Synthesis of High-Quality AFX-type Zeolite Using Bulky and Rigid Organic Structure-Directing Agents and Their Catalytic Applications2017

    • Author(s)
      Y. Kubota
    • Organizer
      IUMRS-ICAM 2017
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Syntetic investigation of MSE- and AFX-type zeolites by using various OSDA and their catalytic application2017

    • Author(s)
      N. Nakazawa, Q. Han, S. Inagaki, Y. Kubota
    • Organizer
      7th FEZA Conference
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 合成法の異なるMSE型ゼオライトの酸触媒特性2016

    • Author(s)
      高野美育,稲垣怜史,窪田好浩
    • Organizer
      第32回ゼオライト研究発表会
    • Place of Presentation
      タワーホール船堀
    • Year and Date
      2016-12-01
    • Related Report
      2016 Annual Research Report
  • [Presentation] 新規骨格ゼオライトYNU-5の合成2016

    • Author(s)
      中澤直人,池田卓史,日吉範人,吉田友香,稲垣怜史,窪田好浩
    • Organizer
      第32回ゼオライト研究発表会
    • Place of Presentation
      タワーホール船堀
    • Year and Date
      2016-12-01
    • Related Report
      2016 Annual Research Report
  • [Presentation] 新規アルミノシリケートゼオライトYNU-5の結晶構造2016

    • Author(s)
      池田卓史,中澤直人,日吉範人,稲垣怜史,窪田好浩
    • Organizer
      第32回ゼオライト研究発表会
    • Place of Presentation
      タワーホール船堀
    • Year and Date
      2016-12-01
    • Related Report
      2016 Annual Research Report
  • [Presentation] Rational seed-directed synthesis of MSE-type zeolites using a simple organic structure-directing agent by extending the composite building unit hypothesis2016

    • Author(s)
      S. Sogukkanli,S.P. Elangovan, 板橋慶治,伊與木健太,高野美育,劉 振東,稲垣怜史,脇原 徹,窪田好浩,大久保達也
    • Organizer
      第32回ゼオライト研究発表会
    • Place of Presentation
      タワーホール船堀
    • Year and Date
      2016-12-01
    • Related Report
      2016 Annual Research Report
  • [Presentation] Al-MCM-68ゼオライト触媒のセリア修飾がDTO反応に及ぼす影響2016

    • Author(s)
      韓 喬,榎枝 築,稲垣怜史,窪田好浩
    • Organizer
      第118回触媒討論会
    • Place of Presentation
      岩手大学
    • Year and Date
      2016-09-21
    • Related Report
      2016 Annual Research Report
  • [Presentation] FAU型前駆体から水熱合成したMSE型ゼオライトの酸触媒特性2016

    • Author(s)
      高野美育,稲垣怜史,窪田好浩
    • Organizer
      第118回触媒討論会
    • Place of Presentation
      岩手大学
    • Year and Date
      2016-09-21
    • Related Report
      2016 Annual Research Report
  • [Presentation] MSE-type zeolite as a nanoporous catalyst for effective formation of light olefins2016

    • Author(s)
      Y. Kubota
    • Organizer
      The 14th International Nanotech Symposium & Nano-Convergence Expo in Korea
    • Place of Presentation
      KINTEX, Goyang, Korea
    • Year and Date
      2016-07-13
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Selective formation of propylene in dimethyl ether-to-olefin reaction over modified MCM-68 zeolite2016

    • Author(s)
      S. Park, S. Inagaki, J.N. Kondo, Y. Kubota
    • Organizer
      18th International Zeolite Conference
    • Place of Presentation
      Rio de Janeiro
    • Year and Date
      2016-06-19
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] MSE-type zeolite as an efficient catalyst for dimethyl ether-to-olefin reaction2015

    • Author(s)
      S. Park, S. Inagaki, Y. Kubota
    • Organizer
      2015 International Chemical Congress of Pacific Basin Societies (Pacifichem 2015)
    • Place of Presentation
      ホノルル
    • Year and Date
      2015-12-15
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] リン修飾したMCM-68 を触媒とするDMEから低級オレフィンへの高効率変換2015

    • Author(s)
      朴成植・稲垣怜史・窪田好浩
    • Organizer
      第116回触媒討論会
    • Place of Presentation
      津
    • Year and Date
      2015-09-16
    • Related Report
      2015 Annual Research Report
  • [Presentation] Preparation of high-performance zeolite catalysts through the control of defect sites2015

    • Author(s)
      Y. Kubota
    • Organizer
      ZMPC2015 - International Symposium on Zeolite and Microporous Crystals 2015
    • Place of Presentation
      札幌
    • Year and Date
      2015-06-28
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Enhanced catalytic performance of dealuminated MCM-68 zeolite in DTO reaction2015

    • Author(s)
      S. Park, S. Inagaki, Y. Kubota
    • Organizer
      ZMPC2015 - International Symposium on Zeolite and Microporous Crystals 2015
    • Place of Presentation
      札幌
    • Year and Date
      2015-06-28
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Selective formation of propylene in dimethyl ether-to-olefin reaction over MCM-68 zeolite2015

    • Author(s)
      S. Park, S. Inagaki, Y. Kubota
    • Organizer
      The 15th Korea-Japan Symposium on Catalysis
    • Place of Presentation
      釜山
    • Year and Date
      2015-05-26
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Book] 高機能ゼオライトの最新技術2015

    • Author(s)
      馬場俊秀
    • Total Pages
      207
    • Publisher
      シーエムシー出版
    • Related Report
      2015 Annual Research Report
  • [Book] ナノ空間材料ハンドブック ―ナノ多孔性材料,ナノ層状物質等が切り開く新たな応用展開2015

    • Author(s)
      有賀克彦,徐 強,木村辰雄,窪田好浩,山内悠輔
    • Total Pages
      548
    • Publisher
      エヌ・ティー・エス
    • Related Report
      2015 Annual Research Report
  • [Remarks] Paper | Kubota Lab.

    • URL

      http://www.kubota.ynu.ac.jp/paper.html

    • Related Report
      2017 Annual Research Report
  • [Remarks] Presentation | Kubota Lab.

    • URL

      http://www.kubota.ynu.ac.jp/presentation.html

    • Related Report
      2017 Annual Research Report 2015 Annual Research Report
  • [Remarks] Kubota Lab.

    • URL

      http://www.kubota.ynu.ac.jp/

    • Related Report
      2016 Annual Research Report
  • [Patent(Industrial Property Rights)] ゼオライトとその製造方法2017

    • Inventor(s)
      窪田好浩、稲垣怜史、中澤直人
    • Industrial Property Rights Holder
      横浜国立大学
    • Industrial Property Rights Type
      特許
    • Filing Date
      2017
    • Related Report
      2017 Annual Research Report
    • Overseas
  • [Patent(Industrial Property Rights)] ゼオライトとその製造方法2016

    • Inventor(s)
      窪田好浩,稲垣怜史,中澤直人
    • Industrial Property Rights Holder
      窪田好浩,稲垣怜史,中澤直人
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2016-191110
    • Filing Date
      2016-09-29
    • Related Report
      2016 Annual Research Report
  • [Funded Workshop] 2015 International Chemical Congress of Pacific Basin Societies (Pacifichem 2015)2015

    • Place of Presentation
      ホノルル
    • Year and Date
      2015-12-15
    • Related Report
      2015 Annual Research Report

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

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