期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2014
卷号：111
期号：23
页码：8357-8362
DOI：10.1073/pnas.1404596111
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：Development of sustainable and biodegradable materials is essential for future growth of the chemical industry. For a renewable product to be commercially competitive, it must be economically viable on an industrial scale and possess properties akin or superior to existing petroleum-derived analogs. Few biobased polymers have met this formidable challenge. To address this challenge, we describe an efficient biobased route to the branched lactone, {beta}-methyl-{delta}-valerolactone ({beta}M{delta}VL), which can be transformed into a rubbery (i.e., low glass transition temperature) polymer. We further demonstrate that block copolymerization of {beta}M{delta}VL and lactide leads to a new class of high-performance polyesters with tunable mechanical properties. Key features of this work include the creation of a total biosynthetic route to produce {beta}M{delta}VL, an efficient semisynthetic approach that employs high-yielding chemical reactions to transform mevalonate to {beta}M{delta}VL, and the use of controlled polymerization techniques to produce well-defined PLA-P{beta}M{delta}VL-PLA triblock polymers, where PLA stands for poly(lactide). This comprehensive strategy offers an economically viable approach to sustainable plastics and elastomers for a broad range of applications.
