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Polyol Structure Influences Enzymatic Hydrolysis of Bio-Based 2,5-Furandicarboxylic Acid (FDCA) Polyesters.
Biotechnology Journal ( IF 4.7 ) Pub Date : 2017-07-22 , DOI: 10.1002/biot.201600741
Karolina Haernvall 1 , Sabine Zitzenbacher 1 , Hassan Amer 2 , Michael T Zumstein 3 , Michael Sander 3 , Kristopher McNeill 3 , Motonori Yamamoto 4 , Michael B Schick 4 , Doris Ribitsch 1 , Georg M Guebitz 1, 5
Affiliation  

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 (Mn ) ranged from 9360-35 800 g mol-1 according to gel permeation chromatography (GPC) analysis. Differential scanning calorimetry (DSC) analyses show decreasing glass transition temperature (Tg ) 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.

中文翻译:

多元醇的结构影响生物基2,5-呋喃二甲酸(FDCA)聚酯的酶促水解。

2,5-呋喃二甲酸的聚酯(FDCA)已引起人们的关注,因为它们可以被视为对苯二甲酸石油基聚酯的生物基替代品。但是,关于基于FDCA的聚酯的生物降解和酶水解知之甚少。这项工作旨在研究不同多元醇对基于FDCA的聚酯的酶促水解的影响。合成了一系列包含各种多元醇的聚酯,并分析了来自Thermobifida cellulosilytica(Thc_Cut1)的角质酶1对酶水解的敏感性。根据凝胶渗透色谱法(GPC)分析,基于FDCA的聚酯的数均分子量(Mn)为9360-35 800 g mol-1。差示扫描量热法(DSC)分析显示,随着二醇链长度的增加,玻璃化转变温度(Tg)降低。除了含有1,6-己二醇,1,8-辛二醇和1,12-十二烷二醇的聚酯,其结晶度分别为27%,37%和30%外,所有聚酯的结晶度均低于1%。Thc_Cut1水解所有测试的聚酯,优先选择含有1,5-戊二醇和1,9-壬二醇的聚酯(57.7±7.5和52.8±4.0%释放的FDCA)。当将直链二醇1,3-丙二醇替换为支链类似物1,2-丙二醇或将乙氧基单元引入聚酯链时,酶活性增加。该结果将有助于扩展基于FDCA的聚酯的微生物生物降解知识。除了含有1,6-己二醇,1,8-辛二醇和1,12-十二烷二醇的聚酯,其结晶度分别为27%,37%和30%外,所有聚酯的结晶度均低于1%。Thc_Cut1水解所有测试的聚酯,优先选择含有1,5-戊二醇和1,9-壬二醇的聚酯(57.7±7.5和52.8±4.0%释放的FDCA)。当将直链二醇1,3-丙二醇替换为支链类似物1,2-丙二醇或将乙氧基单元引入聚酯链时,酶活性增加。该结果将有助于扩展基于FDCA的聚酯的微生物生物降解知识。除了含有1,6-己二醇,1,8-辛二醇和1,12-十二烷二醇的聚酯,其结晶度分别为27%,37%和30%外,所有聚酯的结晶度均低于1%。Thc_Cut1水解所有测试的聚酯,优先选择含有1,5-戊二醇和1,9-壬二醇的聚酯(57.7±7.5和52.8±4.0%释放的FDCA)。当将直链二醇1,3-丙二醇替换为支链类似物1,2-丙二醇或将乙氧基单元引入聚酯链时,酶活性增加。该结果将有助于扩展基于FDCA的聚酯的微生物生物降解知识。Thc_Cut1水解所有测试的聚酯,优先选择含有1,5-戊二醇和1,9-壬二醇的聚酯(57.7±7.5和52.8±4.0%释放的FDCA)。当将直链二醇1,3-丙二醇替换为支链类似物1,2-丙二醇或将乙氧基单元引入聚酯链时,酶活性增加。该结果将有助于扩展基于FDCA的聚酯的微生物生物降解知识。Thc_Cut1水解所有测试的聚酯,优先选择含有1,5-戊二醇和1,9-壬二醇的聚酯(57.7±7.5和52.8±4.0%释放的FDCA)。当将直链二醇1,3-丙二醇替换为支链类似物1,2-丙二醇或将乙氧基单元引入聚酯链时,酶活性增加。该结果将有助于扩展基于FDCA的聚酯的微生物生物降解知识。
更新日期:2019-11-01
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