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Establishment of universal design and synthesis method of functional zeolite by interzeolite conversion using a dual-template method

Research Project

Project/Area Number 16H04218
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Inorganic industrial materials
Research InstitutionHiroshima University

Principal Investigator

Sano Tsuneji  広島大学, 工学研究科, 教授 (80251974)

Co-Investigator(Kenkyū-buntansha) 定金 正洋  広島大学, 工学研究科, 准教授 (10342792)
津野地 直  広島大学, 工学研究科, 助教 (40758166)
Project Period (FY) 2016-04-01 – 2019-03-31
Project Status Completed (Fiscal Year 2018)
Budget Amount *help
¥16,770,000 (Direct Cost: ¥12,900,000、Indirect Cost: ¥3,870,000)
Fiscal Year 2018: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
Fiscal Year 2017: ¥3,380,000 (Direct Cost: ¥2,600,000、Indirect Cost: ¥780,000)
Fiscal Year 2016: ¥11,310,000 (Direct Cost: ¥8,700,000、Indirect Cost: ¥2,610,000)
Keywordsゼオライト / 水熱転換 / 有機構造規定剤 / アンモニウムカチオン / ホスホニウムカチオン / NH3-SCR / 水熱合成 / 混合テンプレート / 多孔体
Outline of Final Research Achievements

We investigated syntheses of small-pore zeoliets such as CHA, AEI and AFX by a mixture of FAU zeolite with high Si/Al ratio and Al source as starting materials. It was found from ESI-MS analysis that a rapid decompsotion of high silica FAU zeolite occurred, giving locally ordered aluminosilicate speceoes (nanoparts) that assembel and evolve into another type of zeolite. Phosphorus-modified small-pore zeolites (CHA, AEI, and LEV) were also prepared by hydrothermal conversion of FAU zeolites with a mixture of an N-OSDA and P-OSDA. These P-modified zeolites exhibit a good catalytic activity and durability in the NH3-SCR process.

Academic Significance and Societal Importance of the Research Achievements

機能性材料ゼオライトを触媒として利用していく際の最大の課題は、構造・組成の安定性に影響する脱アルミニウムをいかに抑制できるかである。deNOx触媒として期待されている小細孔CHA及びAEIゼオライトにおいてホスホニウムカチオンをOSDA及びリン修飾剤とする合成法により、実用化の点からまだ十分と言えるレベルではないが、耐熱/耐水熱安定性を向上できることを明らかにした。ゼオライト合成に関する研究は世界で活発に行われ、筆者らのゼオライト水熱転換法を含む合成技術に関する新たな発見が続いており、高耐久性ゼオライトの設計・合成が近い将来可能になると期待している。

Report

(4 results)
  • 2018 Annual Research Report   Final Research Report ( PDF )
  • 2017 Annual Research Report
  • 2016 Annual Research Report
  • Research Products

    (34 results)

All 2019 2018 2017 2016

All Journal Article (16 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 16 results,  Open Access: 2 results,  Acknowledgement Compliant: 2 results) Presentation (16 results) (of which Int'l Joint Research: 9 results,  Invited: 1 results) Book (2 results)

  • [Journal Article] Zeolite hydrothermal conversion in the presence of various cyclicalkylammonium cations and synthesis of nanosized BEA and MFI zeolites2019

    • Author(s)
      T. Tanigawa, N. Tsunoji, M. Sadakane, T. Sano
    • Journal Title

      Microporous Mesoporous Mater.

      Volume: 277 Pages: 115-123

    • DOI

      10.1016/j.micromeso.2018.10.019

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Comparative study between high-silica faujasites (FAU) from organic-free system and the commercial zeolite Y2019

    • Author(s)
      S. Ferdov, K. Tsuchiya, N. Tsunoji, T. Sano
    • Journal Title

      Microporous Mesoporous Mater.

      Volume: 276 Pages: 154-159

    • DOI

      10.1016/j.micromeso.2018.09.036

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Facile synthesis of highly crystalline EMT zeolite by hydrothermal conversion of FAU zeolite in the presence of 1,1'-(1,4-butanediyl)bis (1-azonia-4-azabicyclo[2,2,2]octane)dihydroxide2019

    • Author(s)
      K. Matsuda, K. Tsuchiya, N. Tsunoji, M. Sadakane, T. Sano
    • Journal Title

      Microporous Mesoporous Mater.

      Volume: 274 Pages: 299-303

    • DOI

      10.1016/j.micromeso.2018.08.036

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Stepwise gel preparation for high-quality CHA zeolite synthesis: A common tool for synthesis diversification2018

    • Author(s)
      Y. Joich, D. Shimono, N. Tsunoji, Y. Takamitsu, M. Sadakane, T. Sano
    • Journal Title

      Cryst. Growth Des.

      Volume: 18 Issue: 9 Pages: 5652-5662

    • DOI

      10.1021/acs.cgd.8b00963

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis of phosphorus-modified AFX zeolite using a dual-template method with tetraethylphosphonium hydroxide as phosphorus modification agent2018

    • Author(s)
      Mitani Emi、Yamasaki Yoshitaka、Tsunoji Nao、Sadakane Masahiro、Sano Tsuneji
    • Journal Title

      Microporous and Mesoporous Materials

      Volume: 267 Pages: 192-197

    • DOI

      10.1016/j.micromeso.2018.03.033

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] リン修飾小細孔ゼオライトの合成とNH3-SCR 触媒特性2018

    • Author(s)
      津野地直、佐野庸治
    • Journal Title

      ゼオライト

      Volume: 35 Pages: 92-100

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 進化するゼオライト合成2018

    • Author(s)
      佐野庸治、津野地直
    • Journal Title

      触媒

      Volume: 60 Pages: 240-246

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] An isomorphously substituted Fe-BEA zeolite with high Fe content: facile synthesis and characterization2018

    • Author(s)
      Y. Naraki, K. Ariga, H. Oka, H. Kurashige, T. Sano
    • Journal Title

      J. Nanosci. Nanotechnol.

      Volume: 18 Pages: 11-19

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] A Collective Case Screening of the Zeolites made in Japan for High Performance NH3-SCR of NOx2018

    • Author(s)
      V. Subramaniam, T. Onishi, Y. Shimada, Y. Kubota, T. Masuda, Y. Nakasaka, M. Matsukata, K. Itabashi, T. Okubo, T. Sano, N. Tsunoji, T. Yokoi, M. Ogura
    • Journal Title

      Bull. Chem. Soc. Jpn.

      Volume: 91 Issue: 3 Pages: 355-361

    • DOI

      10.1246/bcsj.20170352

    • NAID

      130006507116

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Incorporation of various heterometal atoms in CHA zeolites by hydrothermal conversion of FAU zeolite and their performance for selective catalytic reduction of NOx with ammonia2017

    • Author(s)
      Tomoka Takata, Nao Tsunoji, Yasuyuki Takamitsu, Masahiro Sadakane, and Tsuneji Sano
    • Journal Title

      Microporous Mesoporous Mater.

      Volume: 246 Pages: 89-101

    • DOI

      10.1016/j.micromeso.2017.03.018

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] Mesoporous MCM-48 immobilized with aminopropyltriethoxysilane: a potential catalyst for transesterification of triacetin2017

    • Author(s)
      Mahuya Bandyopadhyay, Nao Tsunoji, Tsuneji Sano
    • Journal Title

      Catal. Lett.

      Volume: 147 Issue: 4 Pages: 1040-1050

    • DOI

      10.1007/s10562-017-1997-5

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research / Acknowledgement Compliant
  • [Journal Article] ZTS-1 and ZTS-2: Novel intergrowth zeolites with AFX/CHA structure2017

    • Author(s)
      Y. Naraki, K. Ariga, K. Nakamura, K. Okushita, T. Sano
    • Journal Title

      Microporous Mesoporous Mater.

      Volume: 254 Pages: 160-169

    • DOI

      10.1016/j.micromeso.2017.04.004

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis of phosphorus-modified small-pore zeolites utilizing tetraalkyl phosphonium cations as both structure-directing and phosphorous modification agents2016

    • Author(s)
      Y. Yamasaki, N. Tsunoji, Y. Takamitsu, M. Sadakane, T. Sano
    • Journal Title

      Microporous Mesoporous Mater.

      Volume: 223 Pages: 129-139

    • DOI

      10.1016/j.micromeso.2015.10.038

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] One-pot Synthesis of Phosphorus-modified AEI Zeolites Derived by the Dual-template Method as a Durable Catalyst with Enhanced Thermal/Hydrothermal Stability for Selective Catalytic Reduction of NO<i><sub>x</sub></i> by NH<sub>3</sub>2016

    • Author(s)
      Y. Kakiuchi, Y. Yamasaki, N. Tsunoji, Y. Takamitsu, M. Sadakane, T. Sano
    • Journal Title

      Chemistry Letters

      Volume: 45 Issue: 2 Pages: 122-124

    • DOI

      10.1246/cl.150997

    • NAID

      130005124756

    • ISSN
      0366-7022, 1348-0715
    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Nanosized CHA zeolites with high thermal and hydrothermal stability derived from the hydrothermal conversion of FAU zeolite2016

    • Author(s)
      T.Takata, N.Tsunoji, Y.Takamitsu, M.Sadakane, T.Sano
    • Journal Title

      Microporous Mesoporous Mater.

      Volume: 225 Pages: 524-533

    • DOI

      10.1016/j.micromeso.2016.01.045

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Hydrothermal conversion of titanated FAU to AEI zeolite and its enhanced catalytic performance for NOx reduction2016

    • Author(s)
      N.Funase, T.Takata, N.Tsunoji,, Y.Takamitsu, M.Sadakane, T.Sano
    • Journal Title

      Adv. Porous Mater.

      Volume: 4 Issue: 1 Pages: 62-72

    • DOI

      10.1166/apm.2016.1101

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Presentation] テトラエチルホスホニウム存在下でのFAU-GMEゼオライト水熱転換2018

    • Author(s)
      三谷絵美・津野地直・定金正洋・佐野庸治
    • Organizer
      第34回ゼオライト研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] [Dab-4]2+カチオン存在下におけるFAU-EMTゼオライト水熱転換2018

    • Author(s)
      大西美冴・松田啓吾・土谷和愛・津野地直・定金正洋・佐野庸治
    • Organizer
      第34回ゼオライト研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] ゼオライト合成の多様化を目的とした多段階の合成ゲル調製法の開発とCHAゼオライト合成への応用2018

    • Author(s)
      津野地直・城一洋子・下野大悟・高光泰之・定金正洋・佐野庸治
    • Organizer
      第34回ゼオライト研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 種々なシリカアルミナ源からのAEI型ゼオライトの合成過程の調査とその物性評価2018

    • Author(s)
      下野大悟・城一洋子・高光泰之・津野地直・定金正洋・佐野庸治
    • Organizer
      第34回ゼオライト研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 混合テンプレート法によるAFX/CHA連晶体の合成と高機能化2018

    • Author(s)
      土谷和愛・津野地直・定金正洋・佐野庸治
    • Organizer
      第34回ゼオライト研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] アモルファス原料とSi/Al比の異なる出発FAUゼオライトを様々に組み合わせたCHAゼオライト合成2018

    • Author(s)
      谷川卓也・山崎義貴・津野地直・定金正洋・佐野庸治
    • Organizer
      第34回ゼオライト研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 耐久性ゼオライトの合成―脱アルミニウムとの戦いー2018

    • Author(s)
      佐野庸治
    • Organizer
      第34回ゼオライト研究発表会
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] Synthesis of phosphorus-modified AFX zeolite by the dual-template method with tetraethylphosphonium hydroxide as phosphorus modification agent2018

    • Author(s)
      E. Mitani, Y. Yamasaki, N. Tsunoji, M. Sadakane, T. Sano
    • Organizer
      ZMPC2018
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Control of Si/Al ratio and crystal size of CHA zeolite by combining dealuminated FAU with different Si/Al ratio and additional Si or Al source2018

    • Author(s)
      T. Tanigawa, Y. Yamasaki, N. Tsunoji, M. Sadakane, T. Sano
    • Organizer
      ZMPC2018
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Facile synthesis of highly crystalline EMT zeolite by hydrothermal conversion of FAU zeolite in the presence of 1,1-(1,4-butanediyl) bis(1-azonia-4-azabicyclo[2,2,2]octane) dihydroxide2018

    • Author(s)
      K. Matsuda, K. Tsuchiya, N. Funase, N. Tsunoji, M. Sadakane, T. Sano
    • Organizer
      ZMPC2018
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Rational synthesis of small-pore zeolite through multi-step hydrogel preparation; A common technical tool for high-quality zeolite synthesis2018

    • Author(s)
      D. Shimono, Y. Jyoichi, N. Tsunoji, M. Sadakane, T. Sano
    • Organizer
      ZMPC2018
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Facile ssynthesis of phosphorus-modified small pore zeolites with tetraalkylphosphonium cations and thei NH3-SCR catalytic performance2017

    • Author(s)
      Y.Kakiuchi, Y.Yamasaki, N.Tsunoji, Y.Takamitsu, M.Sadakane, T.Sano
    • Organizer
      7th International FEZA Conference, Sofia, Bulgaria
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Synthesis and characterization of titanated AEI zeolite by hydrothermal conversion of titanated FAU zeolite2017

    • Author(s)
      N.Funase, N.Tsunoji, Y.Takamitsu, M.Sadakane, T.Sano
    • Organizer
      7th International FEZA Conference, Sofia, Bulgaria
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Nanosized CHA zeolite with high thermal/hydrothermal stability derived from hydrothermal conversion of FAU zeolite2016

    • Author(s)
      T.Takata N.Tsunoji, Y.Takamitsu, M.Sadakane, T.Sano
    • Organizer
      18th International Zeolite Conference
    • Place of Presentation
      Rio de Janeiro, Brazil
    • Year and Date
      2016-06-19
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Highly active and selective Ti-incorporated porous silica catalysts derived from grafting of titanium(IV) acetylacetone2016

    • Author(s)
      N.Tsunoji, M.Fukuda, Y.Yagenji, M.Sadakane, T.Sano
    • Organizer
      18th International Zeolite Conference
    • Place of Presentation
      Rio de Janeiro, Brazil
    • Year and Date
      2016-06-19
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Synthesis of phosphorus-modified small-pore zeolites utilizing tetraalkyl phosphonium cations as both structure-directing and phosphorous modification agents2016

    • Author(s)
      Y.Yamasaki, N.Tsunoji, Y.Takamitsu, M.Sadakane,T.Sano
    • Organizer
      18th International Zeolite Conference
    • Place of Presentation
      Rio de Janeiro, Brazil
    • Year and Date
      2016-06-14
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Book] ナノ空間材料2016

    • Author(s)
      津野地直、佐野庸治
    • Total Pages
      999
    • Publisher
      エヌ・ティー・エス
    • Related Report
      2016 Annual Research Report
  • [Book] Encyclopedia of Membranes2016

    • Author(s)
      T.Sano
    • Total Pages
      999
    • Publisher
      Springer-Verlag Berlin Heidelberg
    • Related Report
      2016 Annual Research Report

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Published: 2016-04-21   Modified: 2020-03-30  

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