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戦略的基礎研究推進事業 平成7年度採択研究課題 研究終了報告  873-882
環境低負荷型の高分子物質生産システムの開発
土肥 義治


5年間 (1996-2000) の発表論文(海外81件)
1.ポリエステル生合成の遺伝子工学に関する研究
Biosynthesis of polyesters by recombinant bacteria
(1) M. Kato, T. Fukui and Y. Doi:
Biosynthesis of Polyester Blends by Pseudomonas sp. 61-3 from Alkanoic Acids;
Bull. Chem. Soc. Jpn., 69 515-520 (1996)
(2) Y. Saito, S. Nakamura, M. Hiramitsu and Y. Doi:
Microbial Synthesis and Properties of Poly(3-hydroxybutyrate-co-4-hydroxybutyrate); Polymer Int., 39 169-174 (1996)
(3) M. Kato, H.J. Bao, C.-K. Kang, T. Fukui and Y. Doi:
Production of a Novel Copolyester of 3-Hydroxybutyric Acid and Medium-chain-length 3-Hydroxyalkanoic Acids by Pseudomonas sp. 61-3 from Sugars; Appl. Microbiol. Biotechnol. 45 363-370 (1996)
(4) T. Fukui and Y. Doi:
Cloning and Analysis of the Poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) Biosynthesis Genes of Aeromonas caviae; J. Bacteriol., 179 4821-4830 (1997)
(5) T. Fukui, T. Kichise, Y. Yoshida and Y. Doi:
Biosynthesis of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate-co-3-hydroxyheptanoate) Terpolymers by Recombinant Alcaligenes eutrophus; Biotechnol. Lett., 19 1093-1097 (1997)
(6) M. Kato, T. Fukui, T. Iwata and Y. Doi:
Genetic and Morphological Studies on Biosynthesis of Polyester Blend of Poly(3-hydroxybutyrate) and Poly(3-hydroxybutyrate-co-3-hydroxyalkanoates) in Pseudomonas sp.61-3; “1996 International Symposium on Bacterial Polyhydroxyalkanoates”. Eds by G. Eggink et al., NRC Research Press, 143-150 (1997)
(7) T. Fukui, N. Shiomi and Y. Doi:
Expression and Characterization of (R)-Specific Enoyl Coenzyme A Hydratase Involved in Polyhydroxyalkanoate Biosynthesis by Aeromonas caviae; J. Bacteriol., 180 667-673 (1998)
(8) T. Fukui and Y. Doi:
Efficient Production of Polyhydroxyalkanoates from Plant Oils by Alcaligenes eutrophus and Its Recombinant Strain; Appl. Microbiol. Biotechnol., 49 333-336 (1998)
(9) T. Fukui, M. Kato, H. Matsusaki, T. Iwata and Y. Doi:
Morphological and 13C-Nuclear Magnetic Resonance Studies for Polyhydroxyalkanoate Biosynthesis in Pseudomonas sp. 61-3; FEMS Microbiol. Lett., 164 219-225 (1998)
(10) K. Sudesh, T. Fukui and Y. Doi:
Genetic Analysis of Comamonas acidovorans Polyhydroxyalkanoate Synthase and Factors Affecting the Incorporation of 4-Hydroxybutyrate Monomer; Appl. Environ. Microbiol., 64 3437-3443 (1998)
(11) H. Matsusaki, S. Manji, K. Taguchi, M. Kato, T. Fukui and Y. Doi:
Cloning and Molecular Analysis of the Poly(3-hydroxybutyrate) and Poly(3-hydroxybutyrate-co-3-hydroxyalkanoate) Biosynthesis Genes in Pseudomonas sp. Strain 61-3; J. Bacteriol., 180 6459-6467 (1998)
(12) T. Fukui, S. Yokomizo, G. Kobayashi and Y. Doi:
Co-expression of Polyhydroxyalkanoate Synthase and (R)-Enoyl-CoA Hydratase Genes of Aeromonas caviae Establishes Copolyester Biosynthesis Pathway in Escherichia coli; FEMS Microbiol. Lett., 170 69-75 (1999)
(13) H. Nakashita, Y. Arai, K. Yoshioka, T. Fukui, Y. Doi, R. Usami, K. Horikoshi
and I. Yamaguchi:
Production of Biodegradable Polyester by a Transgenic Tobacco; Biosci. Biotechnol. Biochem., 63 870-874 (1999)
(14) T. Kichise, T. Fukui, Y. Yoshida and Y. Doi:
Biosynthesis of Polyhydroxyalkanoates (PHA) by Recombinant Ralstonia eutropha and Effects of PHA Synthase Activity on in vivo PHA Biosynthesis; Int. J. Biol. Macromol., 25 69-77 (1999)
(15) K. Sudesh, T. Fukui, K. Taguchi, T. Iwata and Y. Doi:
Improved Production of Poly(4-hydroxybutyrate) by Comamonas acidovorans and its Freeze-Fracture Morphology; Int. J. Biol. Macromol., 25 79-85 (1999)
(16) K. Taguchi, Y. Aoyagi, H. Matsusaki, T. Fukui and Y. Doi:
Co-expression of 3-Ketoacyl-ACP Reductase and Polyhydroxyalkanoate Synthase Genes Induces PHA Production in Escherichia coli HB101 Strain; FEMS Microbiol. Lett., 176 183-190 (1999)
(17) K. Taguchi, Y. Aoyagi, H. Matsusaki, T. Fukui and Y. Doi:
Over-Expression of 3-Ketoacyl-ACP Synthase III or Malonyl-CoA-ACP Transacylase Gene Induces Monomer Supply for Polyhydroxybutyrate Production in Escherichia coli HB 101; Biotech. Lett., 21 579-584 (1999)
(18) T. Tsuge, T. Fukui, H. Matsusaki, S. Taguchi, G. Kobayashi, A. Ishizaki, and Y. Doi:
Molecular Cloning of Two (R)-Specific Enoyl-CoA Hydratase Genes from Pseudomonas aeruginosa and Their Use for Polyhydroxyalkanoate Synthesis; FEMS Microbiol. Lett., 184 193-198 (1999)
(19) H. Matsusaki, H. Abe, and Y. Doi:
Biosynthesis and Properties of Poly(3-hydroxybutyrate-co-3-hydroxyalkanoates) by Recombinant Strains of Pseudomonas sp. 61-3; Biomacromolecules, 1 17-22 (2000)
(20) K. Sudesh, T. Fukui, T. Iwata and Y. Doi:
Factors Affecting the Freeze-fracture Morphology of in vivo Polyhydroxyalkanoate Granules; Can. J. Microbiol., 46 304-311 (2000)
(21) H. Matsusaki, H. Abe, K. Taguchi, M. Kato, T Fukui, and Y. Doi:
Biosynthesis of Poly(3-hydroxybutyrate-co-3-hydroxyalkanoates) by Recombinant Bacteria Expressing the PHA Synthesis Gene phaC1 from Pseudomonas sp. 61-3; Appl. Microbiol. Biotechnol., 53 401-409 (2000)
(22) K. Matsumoto, H. Matsusaki, S. Taguchi, M. Seki and Y. Doi:
Cloning and Characterization of the Pseudomonas sp. 61-3 phaG Gene Involved in Polyhydroxyalkanoate Biosynthesis; Biomacromolecules, 2 142-147 (2001)
2.高分子加水分解酵素の構造と機能に関する研究
Structure and function of PHA depolymerases
(23) K. Kasuya, Y. Inoue and Y. Doi:
Adsorption Kinetics of Bacterial PHB Depolymerase on the Surface of Polyhydroxyalkanoate Films; Int. J. Biol. Macromol. 19 35-40 (1996)
(24) Y. Doi, K. Kasuya, H. Abe, N. Koyama, S. Ishiwatari, K. Takagi and Y. Yoshida:
Evaluation of Biodegradabilities of Biosynthetic and Chemosynthetic Polyesters in River Water; Polym. Degrad. Stab., 51 281-286 (1996)
(25) J. Li, J. Uzawa and Y. Doi:
Conformational Behavior of Methyl(3R)-3-{[(3′R)-3′-Hydroxybutanoyl]oxy}butanoate in Solutions: Effect of Intramolecular Hydrogen Bond; Bull. Chem. Soc. Jpn., 70 1887-1893 (1997)
(26) M. Shinomiya, T. Iwata, K. Kasuya and Y. Doi:
Cloning of the Gene for Poly(3-hydroxybutyric acid) Depolymerase of Comamonas testosteroni and Functional Analysis of Its Substrate-Binding Domain; FEMS Microbiol. Lett., 154 89-94 (1997)
(27) K. Kasuya, Y. Inoue, T. Tanaka, T. Akehata, T. Iwata, T. Fukui and Y. Doi:
Biochemical and Molecular Characterization of the Polyhydroxybutyrate Depolymerase of Comamonas acidovorans YM 1609, Isolated from Freshwater; Appl. Environ. Microbiol., 63 4844-4852 (1997)
(28) M. Uefuji, K. Kasuya and Y. Doi:
Enzymatic Degradation of Poly[(R)-3-hydroxybutyrate]: Secretion and Properties of PHB Depolymerase from Pseudomonas stutzeri; Polym. Degrad. Stab., 58 275-281 (1997)
(29) K. Kasuya, K. Takagi, S. Ishiwatari, Y. Yoshida and Y. Doi:
Biodegradabilities of Various Aliphatic Polyesters in Natural Waters; Polym. Degrad. Stab., 59 327-332 (1998)
(30) M. Shinomiya, T. Iwata and Y. Doi:
The Adrorption of Substrate-Binding Domain of PHB Depolymerases to the Surface of Poly(3-hydroxybutyric acid); Int. J. Biol. Macromol., 22 129-135 (1998)
(31) J. Li, J. Uzawa and Y. Doi:
Conformational Analysis of Oligomers of (R)-3-Hydroxybutanoic Acid in Solutions by 1H NMR Spectroscopy; Bull. Chem. Soc. Jpn., 71 1683-1689 (1998)
(32) J. Li, J. Uzawa and Y. Doi:
NMR Spectroscopic Studies on Complex Formation Between Dimeric (R)-3-Hydroxybutanoic Acid and β-Cyclodextrin; Bull. Chem. Soc. Jpn., 71 1953-1957 (1998)
(33) S. Matsumura, Y. Suzuki, K. Tsukada, K. Toshima, Y. Doi and K. Kasuya:
Lipase-Catalyzed Ring-Opening Polymerization of β-Butyrolactone to the Cyclic and Linear Poly(3-hydroxybutyrate); Macromolecules, 31 6444-6449 (1998)
(34) T. Ohura, Y. Aoyagi, K. Takagi, Y. Yoshida, K. Kasuya and Y. Doi:
Biodegradation of Poly(3-hydroxyalkanoic acids) Fibers and Isolation of Poly(3-hydroxybutyric acid)-Degrading Microorganisms under Aquatic Environments; Polym. Degrad. Stab., 63 23-29 (1999)
(35) T. Ohura, K. Kasuya and Y. Doi:
Cloning and Characterization of the Polyhydroxybutyrate Depolymerase Gene of Pseudomonas stutzeri and Analysis of the Function of Substrate-Binding Domains; Appl. Environ. Microbiol., 65 189-197 (1999)
(36) K. Kasuya, T. Ohura, K. Masuda and Y. Doi:
Substrate and Binding Specificities of Bacterial Polyhydroxybutyrate Depolymerases; Int. J. Biol. Macromol., 24 329-336 (1999)
(37) K. Tabata, K. Kasuya, H. Abe, K. Masuda and Y. Doi:
Poly(aspartic acid) Degradation by a Sphingomonas sp. Isolated from Freshwater; Appl. Environ. Microbiol., 65 4268-4270 (1999)
(38) Y. Suzuki, T. Ohura, K. Kasuya, K. Toshima, Y. Doi and S. Matsumura:
Enzyme-catalyzed Ring-opening Polymerization of β-Butyrolactone Using PHB Depolymerase; Chem. Lett., 2000 318-319 (2000)
(39) K. Tabata, H. Abe and Y. Doi:
Microbial Degradation of Poly(aspartic acid) by Two Isolated Strains of Pedobacter sp. and Sphingomonas sp.; Biomacromolecules, 1 157-161 (2000)
(40) K. Kasuya, H. Mitomo, M. Nakahara, A. Aiba, T. Kudo and Y. Doi:
Identification of a Marine Benthic P(3HB)-Degrading Bacterium Isolate and Characterization of Its P(3HB) Depolymerase; Biomacromolecules, 1 194-201 (2000)
(41) T. Hiraishi, T. Ohura, S. Ito, K. Kasuya and Y. Doi:
Function of the Catalytic Domain of Poly(3-hydroxybutyrate) Depolymerase from Pseudomonas stutzeri; Biomacromolecules, 1 320-324 (2000)
3.高分子結晶の構造と機能に関する研究
Structure and enzymatic hydrolysis of polyester crystals
(42) T. Iwata, Y. Doi, K. Kasuya and Y. Inoue:
Visualization of Enzymatic Degradation of Poly[(R)-3-hydroxybutyrate] Single Crystals by an Extracellular PHB Depolymerase; Macromolecules, 30 833-839 (1997)
(43) S. Kusaka, H. Abe, S.Y. Lee and Y. Doi:
Molecular Mass of Poly[(R)-3-hydroxybutyric acid] Produced in a Recombinant Escherichia coli; Appl. Microbiol. Biotechnol., 47 140-143 (1997)
(44) T. Iwata, Y. Doi, T. Tanaka, T. Akehata, M. Shiromo and S. Teramachi:
Enzymatic Degradation and Adsorption on Poly[(R)-3-hydroxybutyrate] Single Crystals with Two Types of Extracellular PHB Depolymerases from Comamonas acidovorans YM 1609 and Alcaligenes faecalis T1; Macromolecules, 30 5290-5296 (1997)
(45) T. Iwata, Y. Doi and J. Azuma:
Direct Imaging of Single Crystals of Regioselectively Substituted Cellulose Heteroesters by Atomic Force Microscopy; Macromolecules, 30 6683-6684 (1997)
(46) T. Iwata and Y. Doi:
Morphology and Enzymatic Degradation of Poly(L-lactic acid) Single Crystals; Macromolecules, 31 2461-2467 (1998)
(47) S. Kusaka, T. Iwata and Y. Doi:
Microbial Synthesis and Physical Properties of Ultra-High-Molecular-Weight Poly[(R)-3-hydroxybutyrate]; J. Macromol. Sci., Pure Appl. Chem., A35 319-335 (1998)
(48) H. Mitomo and Y. Doi:
Lamellar Thickening of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) and Poly(3-hydroxybutyrate-co-4-hydroxybutyrate) by Annealing; Rep. Prog. Polym. Phys. Jpn., 41 239-241 (1998)
(49) S. Kusaka, T. Iwata and Y. Doi;
Properties and Biodegradability of Ultra-High-Molecular-Wight Poly[(R)-3-hydroxybutyrate] Produced by a Recombinant Escherichia coli; Int. J. Biol. Macromol., 25 87-94 (1999)
(50) T. Iwata, Y. Doi, S. Nakayama, H. Sasatsuki and S. Teramachi:
Structure and Enzymatic Degradation of Poly(3-hydroxybutyrate) Copolymer Single Crystals with an Extracellular PHB Depolymerase from Alcaligenes faecalis T1; Int. J. Biol. Macromol., 25 169-176 (1999)
(51) H. Mitomo and Y. Doi:
Lamellar Thickening and Cocrystallization of Poly(hydroxyalkanoate)s on Annealing; Int. J. Biol. Macromol., 25 201-205 (1999)
(52) T. Iwata and Y. Doi:
Enzymatic Degradation of Biosynthetic and Chemosynthetic Polymers; “Biochemical Principles and Mechanisms of Biosynthesis and Biodegradation of Polymers” Ed. by A. Steinbuhel, Wiley-VCH, 214-221 (1999)
(53) T. Iwata and Y. Doi:
Crystal Structure and Biodegradation of Aliphatic Polyester Crystals; Macromol. Chem. Phys., 200 2429-2442 (1999)
(54) T. Iwata, Y. Doi, F. Kokubu and S. Teramachi:
Alkaline Hydrolysis of Solution-Grown Poly[(R)-3-hydroxybutyrate] Single Crystals; Macromolecules, 32 8325-8330 (1999)
(55) T. Iwata and Y. Doi:
Morphology ans Crystal Structure of Solution-Growth Single Crystals of Poly[(R)-3-hydroxyvalerate]; Macromolecules, 33 5559-5565 (2000)
(56) T. Iwata, S. Kusaka and Y. Doi:
Characterization of Ultra-High-Molecular-Weight Poly[(R)-3-hydroxybutyrate] Accumlated in a Recombinant Escherichia Coli and its Biodegradability; ACS Symposium Series; No. 764, Polymer from Renewable Resources: Biopolyesters and Biocatalysis, Chapter 5, 67-76 (2000)
4.生分解性高分子の材料設計に関する研究
Material design of biodegradable polyesters
(57) Y. Furuhashi, T. Iwata, P. Sikorski, E. Atkins and Y. Doi:
Structure and Morphology of the Aliphatic Polyester Poly(β-propiolactone) in Solution-Grown Chain-Folded Lamellar Crystals; Macromolecules, 33 in press (2000)
(58) W.K. Lee, T. Iwata, H. Abe and Y. Doi:
Studies on the Enzymatic Degradation of Solution-Grown Lamellar Crystals of Poly[(R)-3-hydroxybutyrate]: Defects in Crystals; Macromolecules, 33 in press (2000)
(59) Y. Inoue, F. Sano, K. Nakamura, N. Yoshie, Y. Saito, H. Satoh, T. Mino, T. Matsuo
and Y. Doi:
Microstructure of Copoly(3-hydroxyalkanoates) Produced in the Anaerobic-Aerobic Activated Sludge Process; Polymer Int., 39, 183-189 (1996)
(60) M. Ichikawa, K. Nakamura, N. Yoshie, N. Asakawa, Y. Inoue and Y. Doi:
Morphological Study of Bacterial Poly(3-hydroxybutyrate-co-3-hydroxypropionate); Macromol. Chem. Phys., 197 2467-2480 (1996)
(61) N. Koyama and Y. Doi:
Miscibility, Thermal Properties, and Enzymatic Degradability of Binary Blends of Poly[(R)-3-hydroxybutyric acid] with Poly(ε-caprolactone-co-lactide); Macromolecules, 29 5843-5851 (1996)
(62) A. Cao, M. Ichikawa, K. Kasuya, N. Yoshie, N. Asakawa, Y. Inoue, Y. Doi and H. Abe:
Composition Fractionation and Thermal Characterization of Poly(3-hydroxybutyrate-co-3-hydroxypropionate); Polym. J., 28 1096-1102 (1996)
(63) H. Abe and Y. Doi:
Enzymatic and Environmental Degradation of Racemic Poly(3-hydroxybutyric acid)s with Different Stereoregularities; Macromolecules, 29 8683-8688 (1996)
(64) N. Koyama and Y. Doi:
Miscibility of Binary Blends of Poly[(R)-3-hydroxybutyric acid] and Poly[(S)-lactic acid]; Polymer, 38 1589-1593 (1997)
(65) N. Koyama and Y. Doi:
Effects of Solid-State Structures on the Enzymatic Degradability of Bacterial Poly(hydroxyalkanoic acids); Macromolecules, 30 826-832 (1997)
(66) G. Beaucage, S. Rane, S. Sukumaran, M.M. Satkowski, L.A. Schechtman and Y. Doi:
Persistence Length of Isotactic Poly(hydroxy butyrate); Macromolecules, 30 4158-4162 (1997)
(67) Y. Doi and H. Abe:
Structural Effects on Biodegradation of Aliphatic Polyesters; Macromol. Symp., 118 725-731 (1997)
(68) H. Abe, Y. Doi, Y. Hori and T. Hagiwara:
Physical Properties and Enzymatic Degradability of Copolymers of (R)-3-Hydroxybutyric Acid and (S, S) Lactide; Polymer, 39 59-67 (1997)
(69) H. Abe, Y. Doi, H. Aoki and T. Akehata:
Solid-State Structures and Enzymatic Degradabilities for Melt-Crystallized Films of Copolymers of (R)-3-Hydroxybutyric Acid with Different Hydroxyalkanoic Acids; Macromolecules, 31 1791-1797 (1998)
(70) H. Abe, H. Aoki and Y. Doi:
Morphologies and Enzymatic Degradability of Melt-Crystallized Poly(3-hydroxybutyric acid-co-6-hydroxyhexanoic acid); Macromol. Symp., 130 81-89 (1998)
(71) A. Cao, K. Kasuya, H. Abe, Y. Doi and Y. Inoue:
Studies on Comomer Compostional Distribution of the Bacterial Poly(3-hydroxybutyric acid-co-3-hydroxypropionic acid)s and Thermal Characteristrics of their Fractionated Component Copolyesters; Polymer, 20 4801-4816 (1998)
(72) Y. He, T. Masuda, A. Cao, N. Yoshie, Y. Doi and Y. Inoue:
Thermal, Crystallization, and Biodegaradation Behavior of Poly(3-hydroxybutyrate) Blends with Poly(butylene succinate-co-butylene adipate) and Poly(butylene succinate-co-ε-caprolactone); Polym. J., 31 184-192 (1999)
(73) Y. Yoshie, M. Fujiwara, K. Kasuya, H. Abe, Y. Doi and Y. Inoue:
Effect of Monomer Composition and Composition Distribution on Enzymatic Degradation of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate); Macromol. Chem. Phys., 200 977-982 (1999)
(74) H. Abe, Y. Kikkawa, H. Aoki, T. Akehata, T. Iwata and Y. Doi:
Crystallization Behavior and Thermal Properties of Melt-Crystallized Poly[(R)-3-hydroxybutyric acid-co-6-hydroxyhexanoic acid] Films; Int. J. Biol. Macromol., 25 177-183 (1999)
(75) H. Abe and Y. Doi:
Structural Effects on Enzymatic Degradabilities for Poly[(R)-3-hydroxybutyric acid] and Its Copolymers; Int. J. Biol. Macromol., 25 185-192 (1999)
(76) A. Cao, Y. Arai, N. Yoshie. K. Kasuya, Y. Doi and Y. Inoue:
Solid Structure and Biodegradation of the Compositionally Fractionated Poly(3-hydroxybutyric acid-co-3-hydroxypropionic acid)s; Polymer, 40 6821-6830 (1999)
(77) H. Abe, Y. Kikkawa, T. Iwata, H. Aoki, T. Akehata, and Y. Doi:
Microscopic Visualization on Crystalline Morphologies of Thin Films for Poly[(R)-3-hydroxybutyric acid] and its Copolymer; Polymer, 41 867-874 (2000)
(78) I. Ohkoshi, H. Abe, and Y. Doi:
Miscibility and Solid-state Structures for Blends of Poly[(S)-lactide] with Atactic Poly[(R,S)-3-hydroxybutyrate]; Polymer, 41 5985-5992 (2000)
(79) Z. Gan, H. Abe and Y. Doi:
Biodegradable Poly(ethylene succinate) (PES). 1. Crystal Growth Kinetics and Morphology; Biomacromolecules, 1 704-712 (2000)
(80) Z. Gan, H. Abe and Y. Doi:
Biodegradable Poly(ethylene succinate) (PES). 2. Crystal Morphology of Melt-Crystallized Ultrathin Film and Its Change after Enzymatic Degradation; Biomacromolecules, 1 713-720 (2000)