ACIB - Austrian Centre of Industrial Biotechnology GmbH, Konrad Lorenz Strasse 20, 3430, Tulln, Austria.
Division of Chemistry of Renewable Resources, BOKU - University of Natural Resources and Life Sciences, Konrad Lorenz Strasse 24, 3430, Tulln, Austria.
Biotechnol J. 2017 Sep;12(9). doi: 10.1002/biot.201600741. Epub 2017 Aug 10.
Polyesters of 2,5-furandicarboxylic acid (FDCA) have gained attention as they can be regarded as the bio-based alternatives to the petroleum-based polyesters of terephthalic acid. However, only little is known about the biodegradation and enzymatic hydrolysis of FDCA-based polyesters. This work aims to investigate the influence of different polyols on enzymatic hydrolysis of FDCA-based polyesters. A series of polyesters containing various polyols are synthesized and analyzed regarding susceptibility to enzymatic hydrolysis by cutinase 1 from Thermobifida cellulosilytica (Thc_Cut1). FDCA-based polyesters' number average molecular weight (M ) ranged from 9360-35 800 g mol according to gel permeation chromatography (GPC) analysis. Differential scanning calorimetry (DSC) analyses show decreasing glass transition temperature (T ) with increasing diol chain length. Crystallinity of all polyesters is below 1% except for polyesters containing 1,6-hexanediol, 1,8-octanediol, and 1,12-dodecanediol for which calculated crystallinities are 27, 37, and 30%, respectively. Thc_Cut1 hydrolyzes all tested polyesters with preference for polyesters containing 1,5-pentanediol and 1,9-nonanediol (57.7 ± 7.5 and 52.8 ± 4.0% released FDCA). Enzyme activity increases when the linear diol 1,3-propanediol is replaced by the branched analog 1,2-propanediol or ethoxy units are introduced into the polyester chain. The results will contribute to expand the knowledge of microbial biodegradation of FDCA-based polyesters.
2,5-呋喃二甲酸（FDCA）的聚酯由于可以被视为对石油基对苯二甲酸聚酯的生物基替代品而受到关注。然而，人们对 FDCA 基聚酯的生物降解和酶水解知之甚少。本工作旨在研究不同多元醇对 FDCA 基聚酯酶水解的影响。合成了一系列含有不同多元醇的聚酯，并通过纤维素分解菌Thermobifida cellulosilytica 的角质酶 1（Thc_Cut1）分析其对酶水解的敏感性。根据凝胶渗透色谱（GPC）分析，FDCA 基聚酯的数均分子量（M）范围为 9360-35800g/mol。差示扫描量热法（DSC）分析表明，随着二醇链长的增加，玻璃化转变温度（T）降低。除含有 1,6-己二醇、1,8-辛二醇和 1,12-十二二醇的聚酯外，所有聚酯的结晶度均低于 1%，这些聚酯的计算结晶度分别为 27%、37%和 30%。Thc_Cut1 水解所有测试的聚酯，优先水解含有 1,5-戊二醇和 1,9-壬二醇的聚酯（分别释放 57.7±7.5%和 52.8±4.0%的 FDCA）。当线性二醇 1,3-丙二醇被支化类似物 1,2-丙二醇或乙氧基单元取代时，酶活性增加。这些结果将有助于扩展对 FDCA 基聚酯微生物生物降解的认识。
