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Molecular mechanism of liquid-liquid interfacial complexation and development of its function

Research Project

Project/Area Number 12304045
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Research Field 分離・精製・検出法
Research InstitutionOSAKA UNIVERSITY

Principal Investigator

WATARAI Hitoshi  Graduate School of Science, Professor, 大学院・理学研究科, 教授 (30091771)

Co-Investigator(Kenkyū-buntansha) TSUKAHARA Satoshi  Graduate School of Science, Research Associate, 大学院・理学研究科, 助手 (50207338)
FUKUMOTO Takao  Graduate School of Science, Research Associate, 大学院・理学研究科, 助手 (10199268)
MONJUSHIRO Hideaki  Graduate School of Science, Research Associate, 大学院・理学研究科, 助手 (80191071)
渡辺 巌  大阪大学, 大学院・理学研究科, 助教授 (50028239)
Project Period (FY) 2000 – 2002
Project Status Completed (Fiscal Year 2002)
Budget Amount *help
¥45,080,000 (Direct Cost: ¥38,600,000、Indirect Cost: ¥6,480,000)
Fiscal Year 2002: ¥7,280,000 (Direct Cost: ¥5,600,000、Indirect Cost: ¥1,680,000)
Fiscal Year 2001: ¥20,800,000 (Direct Cost: ¥16,000,000、Indirect Cost: ¥4,800,000)
Fiscal Year 2000: ¥17,000,000 (Direct Cost: ¥17,000,000)
Keywordsliquid-liquid interface / Complex formation / Interfacial aggregation / Interfacial molecular recognition / Solvent extraction / Two-phase micro-sheath flow method / Molecular dynamics simulation / Centrifugal liquid membrane method / 錯体生成反応 / 分子認識 / 二相マイクロシーフロー法 / 分子動力学法 / 界面錯形成反応 / 一分子計測 / 拡散ダイナミクス / 超分子科学 / 集合体生成 / 酵素反応 / 界面緩和法 / 蛍光回転緩和
Research Abstract

The aim of this study was to invent new measurement methods of a single molecule behavior and metal complexation kinetics at the liquid-liquid interface and to elucidate the nano property of the interface and the kinetic reaction mechanisms of the complexation. Following useful results were obtained;
1) Evaluation of nanoproperty of the interface by the single molecule probe method
A single fluorescent molecule adsorbed at the interface was chased by a fluorescent microscopy. From observed results, the diffusion coefficient at the interface and the viscosity of the interface was evaluated for the first time. The effect of co-adsorbed surfactant molecules on the single molecule diffusion was also evaluated.
2) Invention of direct measurement method of interfacial reactions
The utility of the centrifugal liquid membrane method was confirmed in various solvent extraction systems. To measure fast interfacial reaction as rapid as a few micro second, a new micro-sheath flow fluorescence microscopy was constructed. Furthermore, a centrifugal liquid membrane/ Raman microscopy and a micro-two phase mass spectrometry were invented.
3) Interfacial catalysis and molecular recognition at the interface
Complexation at the interface was always catalyzed when the adsorption of the ligand or the intermediate complex took place in the process of the reaction. These findings are useful for the design of solvent extraction systems taking into account the catalytic role of the interface. We find out that the aggregation of metal complex was favored at the interface than in bulk phase. Also, the interfacial aggregation exhibited novel molecular recognition ability for nucletic acid bases and diazine isomers.
4) Molecular simulation of the interface
Molecular simulation method was successfully applied for the estimation of the interfacial adsorption energy of ligand.

Report

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

    (63 results)

All Other

All Publications (63 results)

  • [Publications] HASHIMOTO, Fumi: "Lateral Diffusion Dynamics for Single Molecules of Fluorescent Cyanine Dye at Free and Surfactant-Modified Dodecane-Water Interface"Langmuir. (in press).

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] FUJIWARA, Kazuhiko: "Total Internal Reflection Resonance Raman Microspectroscopy for the Liquid/Liquid Interface Ion-Association Adsorption of Cationic Mn(III)-Porphine"Langmuir. 19(7). 2658-2664 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] MONJUSHIRO, Hideaki: "Periodic Expansion-contraction Motion of Photoabsorbing Organic Droplets during Laser Photophoretic Migration in Water"Chem. Lett.. 32(3). 254-255 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] MONJUSHIRO, Hideaki: "Anormalous Laser Photophoretic Behavior of Photo-Absorbing Organic Droplets in Water"Chem. Lett.. 8. 788-789 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] SUWA, Masayori: "Magnetophoretic Velocimetry of Manganese(II) in a Single Microdroplet in a Flow System under a High Gradient Magnetic Field Generated with a Superconducting Magnet"Anal. Chem.. 74(19). 5027-5032 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TSUKAHARA, Satoshi: "Kinetics for Acid-Dissociation of Tetraphenylporphinetetrasulfonate in the Ground State Measured by Laser Photolysis Relaxation Method"Phys. Chem. Chem. Phys.. 4. 1592-1597 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Tadao Furumoto: "Migration Mechanism of Bases and Nucleosides in Oil-in-Water Microemulsion Capillary Electrophoresis"Electrophoresis. 22. 3438-3443 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Kazuhiko Fujiwara: "Axial Hydration and Adsorption of Chloro(5,10,15,20-tetraphenylporphyrinato)manganese(III) at the Toluene/Water Interface, Studied by External Reflection Spectrophotometry"Bull. Chem. Soc. Jpn.. 74. 1885-1890 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] SUWA, Masayori: "Magnetophoretic Velocimetry of Manganese(II) in a Single Emulsion Droplet at the Femtomole Level"Anal. Chem.. 73. 5214-5219 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Hitoshi Watarai: "Molecular dynamics simulation of interfacial adsorption of 2-hydroxy oxime at heptane/water interface"Solv. Extr. Ion Exch.. 19(1). 155-166 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Akira Ohashi: "Direct Spectrophotometric Measurements of Acid-Catalyzed Complexation of Palladium(II) with 2-(5-bromo-2-pyridylazo)-5-diethylaminophenol at the Heptane/Water Interface by a Centrifugal Liquid Membrane Method"Anal. Sci.. 17. 1313-1319 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TOKIMOTO, Takahira: "Microscopic Fluorescence Measurement of Fast Interfacial Complexation by Two-Phase Sheath Flow Method"Chem. Lett.. 3. 204-205 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TSUKAHARA, Satoshi: "Dielectrophoretic Behavior of Single DNA in Planar and Capillary Quadrupole Microelectrodes"Chem. Lett.. 3. 250-251 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] FUJIWARA, Naozumi: "In situ Fluorescence Imaging and Time-Resolved Total Internal Reflection Fluorometry of Palladium(II)-Tetrapyridylporphine Complex Assembled at Toluene-Water Interface"Langmuir. 17(17). 5337-5342 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Yoki Yulizar: "Kinetic Complexation Mechanisms of Ni(II) and Zn(II) with a Pyridylazo-Ligand at Liquid-Liquid Interfaces"Anal. Chim. Acta. 447. 247-254 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Christian Tondre: "Rate of Interfacial Reactions Compared to Bulk Reactions in Liquid-Liquid and Micellar Processes : an Attempt to Clarify a Confusing Situation"J. Colloid Interface Sci.. 243. 1-10 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Akira Ohashi: "Resonance Raman Spectroscopic Detection of Pyridylazo Complex Formed at Liquid-Liquid Interface in Centrifugal Liquid Membrane System"Chem. Lett.. 1238-1239 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Kazuhiko Fujiwara: "Binding of Superoxide Anion with Manganese(III) Tetraphenylporphyrin Complex at the Toluene/Water Interface"Anal. Sci.. 17(Supplement). i1249-i1252 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] FUJIWARA, Naozumi: "Time-Resolved Rotational Anisotropy for Palladium(II)-Tetrapyridylporphine Complex Assemblies Formed at Toluene-Water Interface"Anal. Sci.. 17(Supplement). i231-i234 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] HASHIMOTO, Fumi, TSUKAHARA, Satoshi, WATARAI, Hitoshi: "Single Molecule Detection of Cyanine Dye at the Dodecane-Water Interface"Anal. Sci.. 17(Supplement). i81-i83 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TOKIMOTO, Takahira: "Measurement of Fast Interfacial Complexation Rate by Two-Phase Sheath Flow Laser-Induced Microscopic Fluorometry"Anal. Sci.. 17(Supplement). i1245-i1247 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] YULIZAR, Yoki: "Kinetic study of Ni(II) and Zn(II) complexation with a pyridylazo extraction by a centrifugal liquid membrane method"Anal. Chim. Acta. 419. 107-114 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TSUKAHAYA, Satoshi: "Ligand Dissociation in the Excited State of 2-Thenoyltrifluoroacetonato europium(III) Ion in Aqueous Solution"Chem. Lett.. 412-413 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TSUKAHARA, Satoshi: "Effect of Surfactants on In-Plane and Out-Of-Plane Rotational Dynamics of Octadecylrhodamine B at Toluene-Water Interface"Langmuir. 16(17). 6787-6794 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] HASHIMOTO, Fumi: "Lateral Diffusion Dynamics for Single Molecules of Fluorescent Cyanine Dye at Free and Surfactant-Modified Dodecane-Water Interface"Langmuir. in press.

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] FUJIWARA, Kazuhiko: "Total Internal Reflection Resonance Raman Microspectroscopy for the Liquid/Liquid Interface Ion-Association Adsorptionof Cationic Mn(III)D-Porphine"Langmuir. 19 (7). 2658-2664 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] MONJUSHIRO, Hideaki: "Periodic Expansion-contraction Motion of Photoabsorbing Organic Droplets during Laser Photophoretic Migration in Water"Chem. Lett.. 32(3). 254-255 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] MONJUSHIRO, Hideaki: "Anormalous Laser Photophoretic Behavior of Photo-Absorbing Organic Droplets in Water"Chem. Lett.. (8). 788-789 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] SUWA, Masayori: "Magnetophoretic Vclocimetry of Manganese(II) in a Single Microdroplet in a Flow System under a High Gradient Magnetic Field Generated with a Superconducting Magnet"Anal. Chem.. 74(19). 5027-5032 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TSUKAHARA, Satoshi: "Kinetics for Acid-Dissociation of Tetraphenylporphinetetrasulfonate in the Ground State Measured by Laser Photolysis Relaxation Method."Phys. Chem. Chem. Phys.. 4. 1592-1597 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Tadao Furumoto: "Migration Mechanism of Bases and Nucleosides in Oil-in-Water Microemulsion Capillary Electrophoresis"Electrophoresis. 22. 3438-3443 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Kazuhiko Fujiwara: "Axial Hydration and Adsorption of Chloro(5, 10, 15, 20-tetraphenylporphyrinato) manganese(III) at the Toluene/Water Interface, Studied by External Reflection Spectrophotometry"Bull. Chem. Soc. Jpn.. 74. 1885-1890 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] SUWA, Masayori: "Magnetophoretic Velocimetry of Manganese(II) in a Single Emulsion Droplet at the Femtomole Level"Anal. Chem.. 73. 5214-5219 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Hitoshi Watarai: "Molecular dynamics simulation of interfacial adsorption of 2-hydroxy oxime at heptane/water interface"Solv. Extr. Ion Exch.. 19(1). 155-166 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Akira Ohashi: "Direct Spectrophotometric Measurements of Acid-Catalyzed Complexation of Palladium(II) with 2-(5-bromo-2-pyridylazo)-5-diethylaminophenol at the Heptane/Water Interface by a Centrifugal Liquid Membrane Method"Anal. Sci.. 17. 1313-1319 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TOKIMOTO, Takahira: "Microscopic Fluorescence Measurement of Fast Interfacial Complexation by Two-Phase Sheath Flow Method"Chem. Lett.. (3). 204-205 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TSUKAHARA, Satoshi: "Dielectrophoretic Behavior of Single DNA in Planar and Capillary Quadrupole Microelectrodes"Chem. Lett.. (3). 250-251 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] FUJIWARA, Naozumi: "In situ Fluorescence Imaging and Time-Resolved Total Internal Reflection Fluorometry of Palladium(II)-Tetrapyridylporphine Complex Assembled at Toluene-Water Interface"Langmuir. 17 (17). 5337-5342 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Yoki Yulizar: "Kinetic Complexation Mechanisms of Ni(II) and Zn(II) with a Pyridylazo-Ligand at Liquid-Liquid Interfaces"Anal. Chim. Acta. 447. 247-254 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Christian Tondre: "Rate of Interfacial Reactions Compared to Bulk Reactions in Liquid-Liquid and Micellar Processes: an Attempt to Clarify a Confusing Situation"J. Colloid Interface Sci.. 243. 1-10 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Akira Ohashi: "Resonance Raman Spectroscopic Detection of Pyridylazo Complex Formed at Liquid-Liquid Interface in Centrifugal Liquid Membrane System"Chem. Lett.. 1238-1239 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] Kazuhiko Fujiwara: "Binding of Superoxide Anion with Manganese(III) Tetraphenylporphyrin Complex at the Toluene/Water Interface"Anal. Sci.. 17(Supplement). i1249-i1252 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] FUJIWARA, Naozumi: "Time-Resolved Rotational Anisotropy for Palladium(II)-Tetrapyridylporphine Complex Assemblies Formed at Toluene-Water Interface"Anal. Sci.. 17(Supplement). i231-i234 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] HASHIMOTO, Fumi, TSUKAHARA, Satoshi, WATARAI, Hitoshi: "Single Molecule Detection of Cyanine Dye at the Dodecane-Water Interface"Anal. Sci.. 17(Supplement). i81-i83 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TOKIMOTO, Takahira: "Measurement of Fast Interfacial Complexation Rate by Two-Phase Sheath Flow Laser-Induced Microscopic Fluorometry."Anal. Sci.. 17(Supplement). i1245-i1247 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] YULIZAR, Yoki: "Kinetic study of Ni(II) and Zn(II) complexation with a pyridylazo extraction by a centrifugal liquid membrane method."Anal. Chim. Acta. 419. 107-114 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TSUKAHARA, Satoshi: "Ligand Dissociation in the Excited State of 2-Thenoyltrifluoroacetonato europium(III) Ion in Aqueous Solution"Chem. Lett.. 412-413 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] TSUKAHARA, Satoshi: "Effect of Surfactants on In-Plane and Out-Of-Plane Rotational Dynamics of Octadecylrhodamine B at Toluene-Water Interface"Langmuir. 16(17). 6787-6794 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2002 Final Research Report Summary
  • [Publications] H.Watarai, A.Matsumoto, T.Fukumoto: "Direct electrospray ionization mass spectroscopic measurement of micro-flow oil/water system"Anal. Sci.. 18. 367-368 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] S.Tsukahara, H.Watarai: "Kinetics for acid-dissocation of tetraphenylporphinetetrasulfonate in the ground state measured by laser photolysis relaxation method"Phys. Chem. Chem. Phys.. 4. 1592-1597 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] H.Watarai: "Mass spectrometry and laser-microscopy for the study of interfacial reaction in solvent extraction systems"Proceeding of the International Solvent Extraction Conference. ISEC2002. 64-69 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] A.Ohashi, H.Watarai: "Azo-imine resonance in palladium(II) -pyridylazo complex adsorbed at liquid-liquid interfaces studied by centrifugal liquid membrane-resonance Raman microprobe spectroscopy"Langmuir. 18. 10292-10297 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] H.Watatai: "Molecular dynamics simulation of interfacial adsorption of 2-hydroxy oxime at heptane/water interface"Solv.Extr.Ion.Exch.. 19・1. 155-166 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] T.Tokimoto: "Microscopic fluorescence measurement of fast interfacial complexation by two-phase sheath flow method"Chem.Lett.. 204-205 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] N.Fujiwara: "In sifa fiuorescence imaging and time-resolned total internal reflection fluorometry of Pd(II)-TTP complex assembled of foluene-water interface"Langmuir. 17・17. 5337-5342 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.Fujiwara: "Axial hydration and adsorption of chioro-tpp manganese(III) at the tolueve/water interfaces studiecl by extection reflection spectrophotometry"Bull.Chem.Soc.Jpn. 74. 1885-1890 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] A.Ohashi: "Direct spectrophotometric measurements of acid-catalysed complexation of Pd(II) with 5-Br-PADAP at the heptane/water"Aual.Sci.. 17. 1313-1319 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] C.Tondne: "Rate of interfacial reactions compared to bulk reactions in liquid and liquid and micellar processes"J.Colloid Interface. 243. 1-10 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 渡會 仁: "界面ハンドブック"エヌ・ティー・エス(分担). 10 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] S.Tsukahara: "Ligand dissociation in the excited state of 2-thenoyltrifluoroacetonatoeuropium (III) ion in aqueous solution"Chem.Lett.. 412-413 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] M.Fujiwara: "Construction of an internet compatible database for solvent extraction of metal ions"Solv.Extr.Research Develop.Jpn.. Vol.7. 197-205 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] S.Tsukahara: "Effect of surfactants on in-plane and out-of-plane rotational dynamics of octadecylrhodamine B at toluene-water interface"Langmuir. 16. 6787-6794 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] H.Watarai: "Molecular dynamics simulation of interfacial adsorption of 2-hydroxy oxime at heptane/water interface"Solv.Extr.Ion Exch.. 19(1). 1-121 (2001)

    • Related Report
      2000 Annual Research Report

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Published: 2000-04-01   Modified: 2016-04-21  

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