Enzymes as Green Catalysts for Precision Macromolecular Synthesis

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• 作者：Shin-ichiro Shoda ; Hiroshi Uyama ; Jun-ichi Kadokawa ; Shunsaku Kimura ; Shiro Kobayashi
• 刊名：Chemical Reviews
• 出版年：2016
• 出版时间：February 24, 2016
• 年：2016
• 卷：116
• 期：4
• 页码：2307-2413
• 全文大小：5026K
• 年卷期：
  Shin-ichiro Shoda received his Ph.D. degree from the University of Tokyo in 1981 under the supervision of Professor Teruaki Mukaiyama in the field of synthetic organic chemistry, where he developed the glycosyl fluoride method as a novel glycosylating technology. After spending three years working as an Assistant Professor at the University of Tokyo, he conducted his postdoctoral fellowship at ETH-Zurich (from 1984 until 1986) with Professor Dieter Seebach. In 1986, he moved to Tohoku University and joined the laboratories of Professor Shiro Kobayashi. In 1999, he was promoted to a Full Professor at Tohoku University (Functional Macromolecular Chemistry Laboratory). His research interests include synthesis of carbohydrates, the development of novel glycosylations, macromolecular architecture, and precision synthesis of well-designed functional oligo- and polysaccharides. He received the Award of the Chemical Society of Japan for Young Chemists (1986), the Cellulose Society of Japan Award (2002), and Synthetic Organic Chemistry Award, Japan (2013).
  Hiroshi Uyama obtained his Master Degree of Engineering from Kyoto University in 1987 and subsequently Doctor Degree of Engineering from Tohoku University in 1991 under the direction of Professor Shiro Kobayashi. In 1987 he joined as an Assistant Professor in Tohoku University, thereafter moved to Kyoto University in 1996, and is presently Professor in the Department of Applied Chemistry, Osaka University. He is the recipient of several awards and recognitions, including the Young Scientist Award (Chemical Society of Japan) and the Highest Award of Japan Biotechnology Business Competition. His research interests include biomass plastics and nanoprocessing of polymers.
  Jun-ichi Kadokawa studied applied chemistry and materials chemistry at Tohoku University, where he received his M.S. degree in 1989 and his Ph.D. in 1992 under the supervision of Prof. Shiro Kobayashi. He then joined Yamagata University as a Research Associate. From 1996 to 1997, he worked as a visiting scientist in the research group of Prof. Klaus Müllen at the Max-Planck-Institute for Polymer Research in Germany. In 1999, he became an Associate Professor at Yamagata University and moved to Tohoku University in 2002. He was appointed as a Professor of Kagoshima University in 2004. His research interests focus on enzymatic synthesis of non-natural polysaccharides, new polysaccharide-based materials, and control of the higher-ordered structures of polysaccharides. He received the Award for Encouragement of Research in Polymer Science (1998) and the Cellulose Society of Japan Award (2010).
  Shunsaku Kimura was born in Kyoto, Japan, in 1954. He received his B.S. (1976), M.S. (1978), and Ph.D. (1982, Professor Y. Imanishi) degrees from Kyoto University. He joined the Department of Polymer Chemistry, Kyoto University, as a Research Associate (1981), Lecturer (1992), and Associate Professor (1993). He moved to the Department of Material Chemistry, Kyoto University (1996), and in 1999 he was appointed Full Professor. He spent his postdoctoral career (1982–1984, 1986, Professor R. Schwyzer) at ETH-Zurich, Switzerland. He received the Award of the Society of Polymer Science, Japan, in 1999. He currently serves as Associate Editor for Polymer Journal. His main interests are polymer supramolecular chemistry, peptide engineering, theranostic agents, immune-activating or suppressing materials, and optoelectronics devices.
  Shiro Kobayashi studied organic chemistry and polymer chemistry in Kyoto University, where he received his B.S. and M.S. from Prof. J. Furukawa and Ph.D. from Prof. T. Saegusa in 1969. Then, he worked as a postdoc with Prof. G. A. Olah at Case Western Reserve University for two years. In 1972, he joined Kyoto University as a research associate to start studying polymer synthesis. He stayed as a Humboldt fellow with Prof. H. Ringsdorf at University of Mainz in 1976. Following the lectureship in Kyoto University, he was appointed as a full professor at Tohoku University in 1986, starting research on enzymatic polymerization. In 1997, he moved to Kyoto University and officially retired in 2005, to become Emeritus Professor. Since then, he has been a distinguished professor at Kyoto Institute of Technology. His research interests include polymer synthesis and polymeric materials. In particular, his group developed the enzymatic polymerization, which enabled the first chemical synthesis of natural and unnatural polysaccharides like cellulose, xylan, chitin, hyaluronic acid, chondroitin, various functional polyesters, and new aromatics polymers. The method contributes to green polymer chemistry. He received verious awards among others: the Award of the Chemical Society of Japan for Young Chemists (1976), the Award of the Society of Polymer Science, Japan (1986), Humboldt Research Award, Germany (1999), the Award of the Chemical Society of Japan (2001), the 30th John Stauffer Distinguished Lecture Award in the Sciences, University of Southern California (2002), Medal with Purple Ribbon (2007, Japanese Government), and The Order of the Sacred Treasure, Gold Rays with Neck Ribbon (2015, Japanese Government). He has been a Foreign Member of Northrhine Westfalian Academy of Sciences since 1999. He was a member of the Scientific Advisory Board for the Max Planck Institute for Polymer Research, Mainz (2001–2009). To date, he has served as an editor, regional editor, or honorary editor, and as a member of the (executive) advisory board or editorial (advisory) board for 24 international journals, and currently, he is serving for 8 journals.
• ISSN：1520-6890

文摘

The present article comprehensively reviews the macromolecular synthesis using enzymes as catalysts. Among the six main classes of enzymes, the three classes, oxidoreductases, transferases, and hydrolases, have been employed as catalysts for the in vitro macromolecular synthesis and modification reactions. Appropriate design of reaction including monomer and enzyme catalyst produces macromolecules with precisely controlled structure, similarly as in vivo enzymatic reactions. The reaction controls the product structure with respect to substrate selectivity, chemo-selectivity, regio-selectivity, stereoselectivity, and choro-selectivity. Oxidoreductases catalyze various oxidation polymerizations of aromatic compounds as well as vinyl polymerizations. Transferases are effective catalysts for producing polysaccharide having a variety of structure and polyesters. Hydrolases catalyzing the bond-cleaving of macromolecules in vivo, catalyze the reverse reaction for bond forming in vitro to give various polysaccharides and functionalized polyesters. The enzymatic polymerizations allowed the first in vitro synthesis of natural polysaccharides having complicated structures like cellulose, amylose, xylan, chitin, hyaluronan, and chondroitin. These polymerizations are “green” with several respects; nontoxicity of enzyme, high catalyst efficiency, selective reactions under mild conditions using green solvents and renewable starting materials, and producing minimal byproducts. Thus, the enzymatic polymerization is desirable for the environment and contributes to “green polymer chemistry” for maintaining sustainable society.