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Application of multi-functional mixed-ionic liquid and supercritical CO2 systems for efficient biomass processing

Research Project

Project/Area Number 16H04549
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Properties in chemical engineering process/Transfer operation/Unit operation
Research InstitutionTohoku University

Principal Investigator

SMITH Richard  東北大学, 環境科学研究科, 教授 (60261583)

Co-Investigator(Kenkyū-buntansha) 佐藤 善之  東北大学, 工学研究科, 准教授 (50243598)
平賀 佑也  東北大学, 工学研究科, 学術研究員 (70757814)
Project Period (FY) 2016-04-01 – 2019-03-31
Project Status Completed (Fiscal Year 2018)
Budget Amount *help
¥17,940,000 (Direct Cost: ¥13,800,000、Indirect Cost: ¥4,140,000)
Fiscal Year 2018: ¥1,820,000 (Direct Cost: ¥1,400,000、Indirect Cost: ¥420,000)
Fiscal Year 2017: ¥6,890,000 (Direct Cost: ¥5,300,000、Indirect Cost: ¥1,590,000)
Fiscal Year 2016: ¥9,230,000 (Direct Cost: ¥7,100,000、Indirect Cost: ¥2,130,000)
Keywordsイオン液体 / 物性測定 / 物性理論 / バレロラクトン / 極性 / 超臨界流体
Outline of Final Research Achievements

Mixed-solvents, properties and catalytic systems related to efficient processing of biomass with ionic liquids and supercritical carbon dioxide (scCO2) were studied. Basic physical properties (solute activity coefficients at infinite dilution, high pressure densities and CO2 solubilities) were measured and theoretical relationships were developed. Characterization of solvent polarity was studied by measuring Kamlet-Taft parameters of mixed-solvent systems where it was found that solvent phase polarity could be advantageously controlled with solvent-phase composition. Appropriate catalysts, ionic liquids, supercritical and catalytic systems were identified, whereas hydrogenation of biomass-related substrates with bifunctional catalysts was studied. A hydrogen-free, ionic liquid-scCO2-formic acid-bifunctional Ni/NiO catalyst reaction system that produces gamma-valerolactone in high yields (97%) with unprecedented efficiency (3 h) was developed as one example.

Academic Significance and Societal Importance of the Research Achievements

イオン液体を混合しその両機能を維持しようとする混合イオン液体については世界的にも種々の検討がなされているが,物性研究においてはその検討例が多いとは言えない.実際,本研究にて報告した混合イオン液体へのCO2溶解度や混合イオン液体の無限希釈活量係数については,論文ベースで数報のみしか報告されていない.中でも混合イオン液体の高圧密度については本研究において初めて報告されたものであり,その高圧における非理想性については初めて明らかになった事実である.
混合イオン液体の利用方法は今後もさらなる拡がりを見せると予想され,本研究は非食用バイオマスの有効利用手法構築に向けた重要な位置づけである.

Report

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

    (31 results)

All 2019 2018 2017 2016

All Journal Article (17 results) (of which Peer Reviewed: 17 results,  Acknowledgement Compliant: 2 results) Presentation (12 results) (of which Int'l Joint Research: 8 results,  Invited: 5 results) Book (2 results)

  • [Journal Article] Hydrogen gas-free processes for single-step preparation of transition-metal bifunctional catalysts and one-pot γ-valerolactone synthesis in supercritical CO2-ionic liquid systems2019

    • Author(s)
      Guo Haixin、Hiraga Yuya、Qi Xinhua、Smith Richard Lee
    • Journal Title

      The Journal of Supercritical Fluids

      Volume: 147 Pages: 263-270

    • DOI

      10.1016/j.supflu.2018.11.010

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Measurement and modeling of infinite dilution activity coefficients of organic compounds in an equimolar ionic liquid mixture of [Bmim]Cl and [Bmim][Tf2N]2019

    • Author(s)
      Shida Tomoka、Hiraga Yuya、Sugiyama Takuya、Sato Yoshiyuki、Watanabe Masaru、Smith Richard L.
    • Journal Title

      Fluid Phase Equilibria

      Volume: 488 Pages: 72-78

    • DOI

      10.1016/j.fluid.2019.01.028

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Solvent Polarity of Cyclic Ketone (Cyclopentanone, Cyclohexanone): Alcohol (Methanol, Ethanol) Renewable Mixed-Solvent Systems for Applications in Pharmaceutical and Chemical Processing2018

    • Author(s)
      Duereh Alif、Guo Haixin、Honma Tetsuo、Hiraga Yuya、Sato Yoshiyuki、Lee Smith Richard、Inomata Hiroshi
    • Journal Title

      Industrial & Engineering Chemistry Research

      Volume: 57 Issue: 22 Pages: 7331-7344

    • DOI

      10.1021/acs.iecr.8b00689

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Correspondence between Spectral-Derived and Viscosity-Derived Local Composition in Binary Liquid Mixtures Having Specific Interactions with Preferential Solvation Theory2018

    • Author(s)
      Duereh Alif、Sato Yoshiyuki、Smith Richard Lee、Inomata Hiroshi
    • Journal Title

      The Journal of Physical Chemistry B

      Volume: 122 Issue: 48 Pages: 10894-10906

    • DOI

      10.1021/acs.jpcb.8b09511

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Strategies for using hydrogen-bond donor/acceptor solvent pairs in developing green chemical processes with supercritical fluids2018

    • Author(s)
      Duereh Alif、Smith Richard Lee
    • Journal Title

      The Journal of Supercritical Fluids

      Volume: 141 Pages: 182-197

    • DOI

      10.1016/j.supflu.2017.11.004

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Mechanism of Glucose Conversion into 5-Ethoxymethylfurfural in Ethanol with Hydrogen Sulfate Ionic Liquid Additives and a Lewis Acid Catalyst2018

    • Author(s)
      Guo Haixin、Duereh Alif、Hiraga Yuya、Qi Xinhua、Smith Richard Lee
    • Journal Title

      Energy & Fuels

      Volume: 32 Issue: 8 Pages: 8411-8419

    • DOI

      10.1021/acs.energyfuels.8b00717

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Aspects of solvent polarity and solvent properties in developing efficient systems for processing biomass with ionic liquid mixtures and supercritical CO22018

    • Author(s)
      Yuya Hiraga, Alif Duereh, Richard L. Smith, Jr.
    • Journal Title

      Journal of Supercritical Fluids

      Volume: 134 Pages: 12-20

    • DOI

      10.1016/j.supflu.2017.12.022

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Preface The 30thYear Special issue of the Journal of Supercritical Fluids- Perspectives and Opinions on Current State and Future Directions2018

    • Author(s)
      Erdogan Kiran, Gerd Brunner, Richard L.Smith, Jr., Maria Jose Alonso Cocero, Angela Welch
    • Journal Title

      Journal of Supercritical Fluids

      Volume: 134 Pages: 1-1

    • DOI

      10.1016/j.supflu.2018.02.003

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Measurement and Correlation of High-Pressure Densities and Atmospheric Viscosities of Ionic Liquids: 1-Butyl-1-methylpyrrolidinium Bis(trifluoromethylsulfonyl)imide), 1-Allyl-3-methylimidazolium Bis(trifluoromethylsulfonyl)imide, 1-Ethyl-3-methylimidazolium Tetracyanoborate, and 1-Hexyl-3-methylimidazolium Tetracyanoborate2018

    • Author(s)
      Yuya Hiraga, Saki Hagiwara, Yoshiyuki Sato, Richard L. Smith, Jr.
    • Journal Title

      Journal of Chemical & Engineering Data

      Volume: 印刷中 Issue: 4 Pages: 972-980

    • DOI

      10.1021/acs.jced.7b00773

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Does Synergism in Microscopic Polarity Correlate with Extrema in Macroscopic Properties for Aqueous Mixtures of Dipolar Aprotic Solvents?2017

    • Author(s)
      Alif Duereh, Yoshiyuki Sato, Richard L. Smith, Jr., Hiroshi Inomata, Fabio Pichierri
    • Journal Title

      Journal of Physical Chemistry B

      Volume: 121 Issue: 24 Pages: 6033-6041

    • DOI

      10.1021/acs.jpcb.7b03446

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Perfect recycle and mechanistic role of hydrogen sulfate ionic liquids as additive in ethanol for efficient conversion of carbohydrates into 5-ethoxymethylfurfural2017

    • Author(s)
      Haixin Guo, Alif Duereh, Yuya Hiraga, Taku M. Aida, Xinhua Qi, Richard L. Smith, Jr.
    • Journal Title

      Chemical Engineering Journal

      Volume: 323 Pages: 287-294

    • DOI

      10.1016/j.cej.2017.04.111

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] High pressure densities for mixed ionic liquids having different functionalities: 1-butyl-3-methylimidazolium chloride and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide2017

    • Author(s)
      Y. Hiraga, K. Koyama, Y. Sato, R. L. Smith, Jr.
    • Journal Title

      Journal of Chemical Thermodynamics

      Volume: 108 Pages: 7-17

    • DOI

      10.1016/j.jct.2016.12.037

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Measurement and modeling of CO2 solubility in [bmim]Cl - [bmim][Tf2N] mixed-ionic liquids for design of versatile reaction solvents2017

    • Author(s)
      Y. Hiraga, K. Koyama, Y. Sato, R. L. Smith, Jr.
    • Journal Title

      Journal of Supercritical Fluids

      Volume: 印刷中 Pages: 42-50

    • DOI

      10.1016/j.supflu.2017.02.001

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Journal Article] Measurement of high pressure densities and atmospheric pressure viscosities of alkyl phosphate anion ionic liquids and correlation with the ε*-modified Sanchez-Lacombe equation of state2017

    • Author(s)
      Y. Hiraga, M. Goto, Y. Sato, R. L. Smith, Jr.
    • Journal Title

      Journal of Chemical Thermodynamics

      Volume: 104 Pages: 73-81

    • DOI

      10.1016/j.jct.2016.09.013

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Efficient conversion of fructose into 5-ethoxymethylfurfural with hydrogen sulfate ionic liquids as co-solvent and catalyst2017

    • Author(s)
      H. Guo, X. Qi, Y. Hiraga, T. M. Aida, R. L. Smith, Jr.
    • Journal Title

      Chemical Engineering Journal

      Volume: 314 Pages: 508-514

    • DOI

      10.1016/j.cej.2016.12.008

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Methodology for Replacing Dipolar Aprotic Solvents Used in API Processing with Safe Hydrogen-Bond Donor and Acceptor SolventPair Mixtures2017

    • Author(s)
      A. Duereh, Y. Sato, R. L. Smith, Jr., H. Inomata
    • Journal Title

      Organic Process Research & Development

      Volume: 21 Issue: 1 Pages: 114-124

    • DOI

      10.1021/acs.oprd.6b00401

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Measurement and modeling of adsorption equilibria of imidazolium-based ionic liquids on activated carbon from aqueous solutions2017

    • Author(s)
      I. Ushiki, M. Tashiro, R. L. Smith, Jr.
    • Journal Title

      Fluid Phase Equilibria

      Volume: 印刷中 Pages: 17-23

    • DOI

      10.1016/j.fluid.2017.01.021

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Presentation] Measurement and modeling of infinite dilution activity coefficients for organic compounds in ionic liquid mixtures ([Bmim]Cl0.50[Tf2N]0.50)2018

    • Author(s)
      Tomoka Shida, Yuya Hiraga, Takuya Sugiyama, Yoshiyuki Sato, Masaru Watanabe, Richard L. Smith, Jr.
    • Organizer
      Molecular Thermodynamics and Molecular Simulation (MTMS '18)
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] CO2添加によるリン酸系混合イオン液体のH2溶解度増進効果に関する研究2018

    • Author(s)
      萩原 沙樹,平賀 佑也,佐藤 善之,相田 卓,渡邉 賢,Richard L. Smith, Jr.
    • Organizer
      化学工学会 第83年会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Methodology of using mixed-solvents for developing green chemical processes2017

    • Author(s)
      Richard L. Smith, Jr.
    • Organizer
      The 5th International Symposium & Exhibition on Aqua Science and Water Resources (ISASWR'17)
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Measurement and Modeling of Kamlet-Taft Solvatochromic Parameters of Hydrogen-Bond donor and Acceptor Solvent Mixtures with the Preferential Solvation Model2017

    • Author(s)
      Yuya Hiraga, Haixin Guo, Yoshiyuki Sato, Richard L. Smith, Jr.
    • Organizer
      The 5th International Symposium & Exhibition on Aqua Science and Water Resources (ISASWR'17)
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Stability of 5-hydroxymethylfurfural in the mixture of hydrogen sulfate ionic liquid and ethanol2017

    • Author(s)
      Haixin Guo, Alif Duereh, Taku M. Aida, Richard L. Smith, Jr.
    • Organizer
      The 5th International Symposium & Exhibition on Aqua Science and Water Resources (ISASWR'17)
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Strategies for Using Mixed-solvents in Supercritical Fluid Science and Technology2017

    • Author(s)
      Alif Duereh, Yuya Hiraga, Richard L. Smith, Jr.
    • Organizer
      6th European Meeting on Supercritical Fluids (EMSF)
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Aspects of mixed-solvents for reactions and separations2016

    • Author(s)
      R. L. Smith, Jr.
    • Organizer
      平成28年度化学系学協会東北大会
    • Place of Presentation
      いわき明星大学(福島・いわき)
    • Year and Date
      2016-09-10
    • Related Report
      2016 Annual Research Report
    • Invited
  • [Presentation] Partition coefficients of benzene derivatives in ionic liquid - CO2 biphasic systems2016

    • Author(s)
      Y. Hiraga, Y. Sato, R. L. Smith, Jr.
    • Organizer
      平成28年度化学系学協会東北大会
    • Place of Presentation
      いわき明星大学(福島・いわき)
    • Year and Date
      2016-09-10
    • Related Report
      2016 Annual Research Report
  • [Presentation] イミダゾリウム系イオン液体へのH2およびH2+CO2混合ガス溶解度に関する研究2016

    • Author(s)
      萩原沙樹,後藤武蔵,平賀佑也,佐藤善之,相田卓,渡邉賢,スミスリチャード
    • Organizer
      化学工学会第48回秋季大会
    • Place of Presentation
      徳島大学(徳島・徳島)
    • Year and Date
      2016-09-06
    • Related Report
      2016 Annual Research Report
  • [Presentation] Replacement of toxic solvents used in the pharmaceutical industry with safe and renewable mixed-solvents2016

    • Author(s)
      R. L. Smith, Jr.
    • Organizer
      International Conference on Industrial Pharmacy 2016
    • Place of Presentation
      Kuantan (Malaysia)
    • Year and Date
      2016-08-14
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Theoretical Analysis of ePC-SAFT Equation of State for Predicting Infinite Dilution Partition Coefficients in Supercritical CO2 - Ionic Liquid Biphasic Systems2016

    • Author(s)
      Y. Hiraga, Y. Sato, R. L. Smith, Jr.
    • Organizer
      14th PPEPPD 2016 (International Conference on Properties and Phase Equilibria for Product and Process Design)
    • Place of Presentation
      Porto (Portugal)
    • Year and Date
      2016-05-22
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] High Pressure PVT and Solubility of Supercritical CO2 in Mixed Ionic Liquids having Different Functionalities2016

    • Author(s)
      Y. Hiraga, K. Koyama, M. Goto, Y. Sato, R. L. Smith, Jr.
    • Organizer
      15th European Meeting on Supercritical Fluids (EMSF)
    • Place of Presentation
      Essen (Germany)
    • Year and Date
      2016-05-08
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research / Invited
  • [Book] Production of Platform Chemicals from Sustainable Resources2017

    • Author(s)
      Zhen Fang, Richard L. Smith, Jr., Xinhua Qi
    • Total Pages
      475
    • Publisher
      Springer Singapore
    • ISBN
      9789811041723
    • Related Report
      2017 Annual Research Report
  • [Book] Production of Biofuels and Chemicals with Bifunctional Catalysts2017

    • Author(s)
      Zhen Fang, Richard L. Smith, Jr., Hu Li
    • Total Pages
      391
    • Publisher
      Springer Singapore
    • ISBN
      9789811051371
    • Related Report
      2017 Annual Research Report

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

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