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Study on Volume-Phase Transition in Polyelectrolyte Gels at the Molecular Level

Research Project

Project/Area Number 11305066
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Research Field 高分子構造・物性(含繊維)
Research InstitutionUniversity of Tsukuba

Principal Investigator

KOKUFUTA Etsuo  University of Tsukuba, Institute of Applied Biochemistry, Professor, 応用生物化学系, 教授 (40124648)

Co-Investigator(Kenkyū-buntansha) 吉田 亮  筑波大学, 応用生物化学系, 講師 (80256495)
Project Period (FY) 1999 – 2002
Project Status Completed (Fiscal Year 2002)
Budget Amount *help
¥33,300,000 (Direct Cost: ¥31,200,000、Indirect Cost: ¥2,100,000)
Fiscal Year 2002: ¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
Fiscal Year 2001: ¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
Fiscal Year 2000: ¥8,400,000 (Direct Cost: ¥8,400,000)
Fiscal Year 1999: ¥15,800,000 (Direct Cost: ¥15,800,000)
KeywordsPolyelectrolytes Gels / Charge Distribution / Swelling Force / Electrostatic Repulsion / Hydrophobic Interaction / Hydrogen Bonding / Flory's Model / Katchalsky's Model / 体積相転移 / Flory-Huggins理論 / 分子間相互作用 / クーロン斥力 / クーロン引力 / クローン斥力 / クローン引力
Research Abstract

The purpose of this study is to experimentally demonstrate that the volume-phase transition in polyelectrolyte gels can be explained by our hypothesizing balance model (F. Ilmain, T. Tanaka, E. Kokufuta, Nature, 349, 400-401 (1991)). In this model, the transition is accounted for by hypothesizing a balance between the repulsion and attraction among functional groups attached to the network which arise from a combination of four interrmolecular forces : ionic, hydrophobic, van der Waals and hydrogen bonding. When a repulsive force, usually electrostatic in nature, overcomes an attractive force such as hydrogen bonding or hydrophobic interaction, the gel volume should increase discontinuously in some cases and continuously in others. The variables that trigger the transition influence these intermolecular forces and thereby the balanced state of the attractive and repulsive forces. We thus focused on the effect of charge distributions on the swelling of polyelectrolyte gels. Our gel samp … More les ranged from the usual bulk gel to nano-sized particles in shape. The charge distribution within the gel phase was created by different ways : binding of ionic surfactants, physical entrapment of polyions ; and immobilized enzyme reaction. It has became apparent that an charge inhomogeneity plays an important role in the swelling of ionic gels which takes place when the repulsion among the polymer-bound negative or positive charges overcomes hydrogen bonding and/or hydrophobic interaction as the attractive force. This is not able to explain in terms of Flory's model based on net osmotic pressure arising from mobile ions. The conclusions obtained from the present study have been applied in the construction of 〓biochemo-mechanical systems〓 capable of converting biochemical energy created as a result of an immobilized enzyme reaction into mechanical work through the swelling and shrinking of the gel. In addition, polyelectrolyte nanogel particles with diameters in the range of tens to hundreds of nanometers have been designed and synthesized on the basis of the present conclusions. Less

Report

(5 results)
  • 2002 Annual Research Report   Final Research Report Summary
  • 2001 Annual Research Report
  • 2000 Annual Research Report
  • 1999 Annual Research Report
  • Research Products

    (57 results)

All Other

All Publications (57 results)

  • [Publications] E.Kokufuta: "Phase Transitions in Polyelectrolyte Gels"Physical Chemistry of Polyelectrolytes (Surfactant Science Series, Vol.99)(Marcel Dekker, Inc.). 74 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] H.Suzuki, E.Kokufuta: "Inhomogeneous Binding of Ionic Surfactants o Bulk Gels and Microgels Consisting of Poly (N-isopropylacrylamide)"Colloids and Surfaces A. 147. 233-240 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] S.Ito, K.Ogawa, H.Suzuki, B.Wang, R.Yoshida, E.Kokufuta: "Preparation of Thermosensitive Submicron Gel Particles with Anionic and Cationic Charges"Langmuir. 15. 4289-4294 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] H.Suzuki, B.Wang, R.Yoshida, E.Kokufuta: "Potentiometric Titration Behaviors of Polymer and Gel Consisting of N-Isopropylacrylamide and Acrylic Acid"Langmuir. 15. 4283-4288 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] R.Yoshida, M.Tanaka, S.Onodera, T.Yamaguchi, E.Kokufuta: "In-Phase Synchronization of Chemical and Mechanical Oscillations in Self-Oscillating Gels"J. Phys. Chem. A. 104. 7549-7555 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Y.Ogawa, K.Ogawa, B.Wang, E.Kokufuta: "A Biochemo-Mechanical System Consisting of Polyampholyte Gels with Coimmobilized Glucose Oxidase and Urease"Langmuir. 17. 2670-2674 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K.Ogawa, B.Wang, E.Kokufuta: "Enzyme Regulated Microgel Collapse for Controlled Membrane Permeability"Langmuir. 17. 4704-4707 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K.S.Schmitz, B.Wang, E.Kokufuta: "Mechanism of Microgel Formation via Crosslinking of Polymers in Their Dilute Solutions : Mathematical Explanation with Computer Simulations"Macromolecules. 34. 8370-8377 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K.Ogawa, T.Nakajima-Kambe, T.Nakahara, E.Kokufuta: "Coimmobilization of Gluconolactonase with Glucose Oxidase for Improvement in Kinetic Property of Enzymatically Induced Volume Collapse in Ionic Gels"Biomacromolecules. 3. 625-631 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K.Ogawa, E.Kokufuta: "Enzymatic Formation of pH Gradients within Polyelectrolyte Gels with Immobilized Urease"Langmuir. 18. 5661-5667 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K.Ogawa, Y.Ogawa, E.Kokufuta: "Effect of charge inhomogeneity of polyelectrolyte gels on their swelling behavior"Colloids & Surfaces A : Physicochemical and Engineering Aspects. 209. 267-279 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K.Ogawa, E.Kokufuta: "Formation of a Charge Distribution within Ionic Gels by Immobilized Enzyme Reaction : Experimental Observations and Mathematical Simulations"Macromolecular Symposia. (in press). (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K.Ogawa, A.Nakayama, E.Kokufuta: "Preparation and Characterization or Thermosensitive Polyampholyte Nanogels"Langmuir. 19. 3178-3184 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] H. Suzuki, E. Kokufuta: "Inhomogeneous Binding of Ionic Surfactants to Bulk Gels and Microgels Consisting of Poly(N-isopropylacrylamide)"Colloids and Surfaces A. 147[1-2]. 233-240 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] S.Ito, K. Ogawa, H Suzuki, B Wang, R. Yoshida, E. Kokufuta: "Preparation of Thermosensitive Submicron Gel Particles with Anionic and Cationic Charges"Langmuir. 15[12]. 4289-4294 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] H. Suzuki, B. Wang, R. Yoshida, E. Kokufuta: "Potentiometric Titration Behaviors of Polymer and Gel Consisting of N-Isopropylacrylamide and Acrylic Acid"Langmuir. 15[12]. 4283-4288 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] R. Yoshida, M. Tanaka, S.Onodera, T. Yamaguch, E. Kokufuta: "In-Phase Synchronization of Chemical and Mechanical Oscillations in Self-Oscillating Gels"J. Phys. Chem A. 104[32]. 7549-7555 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Y. Ogawa, K. Ogawa, B. Wang, E. Kokufuta: "A Biochemo-Mechanical System Consisting of Polyampholyte Gels with Coimmobilized Glucose Oxidase and Urease"Langmuir. 17[9]. 2670-2674 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K. Ogawa, B. Wang, E. Kokufuta: "Enzyme Regulated Microgel Collapse for Controlled Membrane Permeability"Langmuir. 17[16]. 4704-4707 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K. S. Schmitz, B. Wang, E. Kokufuta: "Mechanism of Microgel Formation via Crosslinking of Polymer in Their Dilute Solutions : Mathematical Explanation with Computer Simulations"Macromolecules. 34[23]. 8370-8377 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K. Ogawa, T. Nakajima-Kambe, T. Nakahara, E. Kokufuta: "Coimmobilization of Gluconolactonase with Glucose Oxidase for Improvement in Kinetic Property of Enzymatically Induced Volume Collapse in Ionic Gels"Biomacromolecules. 3[3]. 625-631 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K. Ogawa, E. Kokufuta: "Enzymatic Formation of pH Gradients within Polyelectrolyte Gels with Immobilized Urease"Langmuir. 18[15]. 5661-5667 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K. Ogawa, Y. Ogawa, E. Kokufuta: "Effect of charge inhomogeneity of polyelectrolyte gels on their swelling behavior"Colloids & Surfaces A : Physicochemical and Engineering Aspects. 209[2/3]. 267-279 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K. Ogawa, E. Kokufuta: "Formation of a Charge Distribution within Ionic Gels by Immobilized Enzyme Reaction : Experimental Observations and Mathematical Simulations"Macromolecular Symposia. in press. (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K. Ogawa, A. Nakayama, E. Kokufuta: "Preparation and Characterization of Thermosensitive Polyampholyte Nanogels"Langmuir. 19[8]. 3178-3184 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] E. Kokufuta , ed. by T.Radeva: "Phase Transitions in Polyelectrolyte Gels In : Physical Chemistry of Polyelectrolytes (Surfactant Science Series)"Marcel Dekker, Inc.. 99 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] K.Ogawa, Y.Ogawa, E.Kokufuta: "Effect of Charge Inhomogeneity of Polyelectrolyte Gels on Their Swelling Behavior"Colloid. & Surf., A. 209・2. 267-279 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] K.Ogawa, E.Kokufuta: "Enzymatic Formation of pH Gradients within Polyelectrolyte Gels with Immobilized Urease"Langmuir. 18・15. 5661-5667 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] K.Ogawa, T.Nakajima-Kambe, T.Nakahara, E.Kokufuta: "Coimmobilization of Glouconolactonase with Glucose Oxidase for Improvement in Kinetic Property of Enzymatically Induced Volume Collapse in Ionic Gels"Biomacromolecules. 3・3. 625-631 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] O.Tabata, H.Hirawawa, S.Aoki, R.Yoshida, E.Kokufuta: "Ciliary Motion Actuator Using Self-oscillating Gel"Sensors & Actuators, A. 95・2. 234-238 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] T.Norisuye, N.Masui, Y.Kida, D.Ikuta, E.Kokufuta, Shoji Ito, S.Panyukov, Mitsuhiro Shibayama: "Small Angle Neutron Scattering Studies on Structural Inhomogeneities in Polymer Gels : Irradiation Cross-linked Gels vs Chemically Cross-linked Gels"polymer. 43・6. 5289-5297 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] K.Ogawa, A.Nakayama, E.Kokufuta: "preparation and Characterization of Thermosensitive Polyampholyte Nanogels"Langmuir. 19(印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] E.Kokufuta: "Smart Polymer for Bioseparation and Bioprocessing"Taylor & Francis Publishers. 520 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] Y.Ogawa, K.Ogawa, B.Wang, E.Kokufuta: "A Biochemo-Mechanical System Consisting of Polyampholyte Gels with Coimmobilized Glucose Oxidase and Urease"Langmuir. 17・9. 2670-2674 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Ogawa, B.Wang, E.Kokufuta: "Enzyme Regulated Microgel Collapse for Controlled Membrane Permeability"Langmuir. 17・16. 4704-4707 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.S.Schmitz, B.Wang, E.Kokufuta: "Mechanism of Microgel Formation via Crosslinking of Polymers in Their Dilute Solutions: Mathematical Explanation with Computer Simulations"Macromolecules. 34・23. 8370-8377 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Yabusaki, E.Kokufuta: "Aggregation Mechanism of Blood Platelets by Time-Resolved Light Scattering Method"Langmuir. 18・1. 39-45 (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Ogawa, E.Kokufuta: "Enzymatic Formation of pH Gradients within Polyelectrolyte Gels with Immobilized Urease"Langmuir. 18(印刷中). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Ogawa, Y.Ogawa, E.Kokufuta: "K.Ogawa, Y.Ogawa, E.Kokufuta:Effect of Charge Inhomogeneity of Polyelectrolyte Gels on Their Swelling Behavior"Colloid. & Surf., A. 150(印刷中). (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] E.Kokufuta: "Physical Chemistry of Polyelectrolytes"Marcel Dekker,Inc. 882 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] B.Wang,S.Mukataka,E.Kokufuta,M.Ogiso,M.Kodama :: "Viscometric, Light Scattering, and Size-Exclusion Chromatography Studies on the Structural Changes of Aqueous Poly (vinyl alcohol) Induced by γ-Ray Irradiation"J.Polym.Sci., Polym Phys.Edn.Part B.Polymer Physics. 38・1. 214-221 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] B.Wang,S.Mukataka,E.Kokufuta,M.Kodama: "The Influence of Polymer Concentration on the Radiation-Chemical Yield of Intermolecular Crosslinking of Poly (vinyl alcohol) by γ-Rays in Deoxygenated Aqueous Solution"Radiat.Phys.Chem.. 59・1. 91-95 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] R.Yoshida,T.Yamaguchi,E.Kokufuta: "Self-Oscillation Mechanism of Hydrogel Coupled with Chemical Oscillations"Macromolc.Symp.. 60・1. 183-189 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] R.Yoshida,M.Tanaka,S.Onodera,T.Yamaguch,E.Kokufuta: "In-Phase Synchronization of Chemical and Mechanical Oscillations in Self-Oscillating Gels"J.Phys.Chem.A. 104・32. 7549-7555 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] 国府田悦男: "ゲルの機能とマテリアルライフ;刺激応答性ゲルを中心として"マテリアルライフ. 12・4. 171-179 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Y.Ogawa,K.Ogawa,B.Wang,E.Kokufuta: "A Biochemo-Mechanical System Consisting of Polyampholyte Gels with Coimmobilized Glucose Oxidase and Urease"Langmuir. (印刷中). (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] B.Wang.E.Kokufuta: "Advances in Crystal Growth Inhibition Technogogies"Kluwer Academic / Plenum Publisheres. 235-254 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] E.Kokufuta: "Physical Chemistry of Polyelectrolytes"Marcel Dekker.Inc(印刷中). (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Suzuki,E.Kokufuta: "Inhomogeneous Binding of Ionic Surfactants to Bulk Gels and Microgels Consisting of Poly(N-isopropylacrylamide)"Colloids and Surfaces A. 147・3. 233-240 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] E.Kokufuta,H.Suzuki,R.Yoshida,F.Kaneko,K.Yamada,M.Hirata: "Volume Collapse of a Cationic Poly(ehtyleneimine)Gel Induced by the Binding of Anionic Surfactants"Colloids and Surfaces A. 147・3. 179-187 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] H.Suzuki,B.Wang,R.Yoshida,and E.Kokufuta: "Potentiometric Titration Behaviore of Polymer and Gel Consisting of N-Isopropylacrylamide and Acrylic Acid"Langmuir. 15・12. 4289-4294 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] S.Ito,K.Ogawa,H.Suzuki,B.Wang,R.Yoshida,E.Kokufuta: "Preparation of Thermosensitive Submicron Gel Particles with Anionic and Cationic Charges"Langmuir. 15・12. 4283-4288 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] E.Kokufuta: "Polyelectrolyte-coated Microcapsules and Their Potential Applications to Biotechnology"Bioseparation. 7・2. 241-252 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] R.Yoshida,S.Onodera,T.Yamaguchi,E.Kokufuta: "Aspects of the Belousov-Zhabotinsky Reaction in Polymer Gels"J.Phys.Chem.A. 103・43. 8573-8578 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] R.Yoshida,T.Yamaguchi,E.Kokufuta: "New Inteligent Polymer Gel: A Self-oscillating Gel with Peacemaking and Actuating Functions"J.Artif.Organs. 2・2. 135-140 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] 国府田悦男、小川和義: "刺激応答性ゲル:10年間の研究動向"高分子. 48・6. 404-407 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] 国府田悦男: "ゲルを用いたバイオケモメカニカルシステムの構築"機能材料. 19・1. 51-61 (1999)

    • Related Report
      1999 Annual Research Report

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Published: 1999-04-01   Modified: 2016-04-21  

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