Xinming Zheng, Jundan Feng, Yuzheng Lu, Rong Li, Artur Cavaco-paulo, Jiajia Fu
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引用次数: 0
Abstract
Enzymatic hydrolysis of polyethylene terephthalate (PET) for surface modification of polyester fibers has attracted considerable research attention in recent years. However, the high crystallinity of polyester fibers, combined with limited enzyme activity and stability, challenges the surface modification study of enzymes. Deep eutectic solvents (DES) can create a favorable environment for proteins and are a new generation of biodegradable solvents. Few studies have been conducted on the use of DES to enhance enzymatic degradation. Therefore, we attempted to hydrolyze PET with DES-activated enzymes to increase the hydrolysis yield and thus improve PET modification. Using betaine and choline chloride as hydrogen bond acceptors and polyols as hydrogen bond donors, we investigated the effects of DES type, molar ratio, and concentration on enzymatic hydrolysis. Humicola insolens cutinase (HiC) was used as the biocatalyst for PET fabric hydrolysis, the role of DES as an additive in improving the yield of enzymatically hydrolyzed PET fabric was investigated. The results showed that under the conditions of an enzyme concentration of 6.5% v/v (volume of enzyme on the total volume), a temperature of 60 °C, and a reaction time of 72 h, the low concentration (20% v/v) of DES (betaine: sorbitol; 1:2 molar ratio) increased the hydrolysis yield by more than 1.5 times. Enzymatic hydrolysis in DES aqueous solution (betaine: sorbitol; 1:2 molar ratio) and DES single-component aqueous solution (betaine, sorbitol without synthesis of DES) indicated that the increase in hydrolysis yield was mainly due to the formation of hydrogen bonds between betaine and sorbitol, rather than the superposition of individual components. Further analysis revealed that HiC exhibited high relative enzyme activity and stability at low DES concentrations. Additionally, CD spectroscopy and fluorescence spectroscopy analyses demonstrated the effective preservation of HiC structure by DES. Our work provides insights into the development of efficient and sustainable methods to enhance HiC hydrolysis of PET fabric, unlocking new opportunities and potential for the comprehensive utilization of DES in the bio-modification of PET fabric.
近年来，用于聚酯纤维表面改性的聚对苯二甲酸乙二酯（PET）酶水解引起了相当多的研究关注。然而，聚酯纤维的结晶度高，加之酶的活性和稳定性有限，给酶的表面改性研究带来了挑战。深共晶溶剂（DES）能为蛋白质创造有利的环境，是新一代的生物可降解溶剂。利用 DES 促进酶降解的研究很少。因此，我们尝试用 DES 激活的酶水解 PET，以提高水解产率，从而改善 PET 的改性。我们使用甜菜碱和氯化胆碱作为氢键受体，多元醇作为氢键供体，研究了 DES 类型、摩尔比和浓度对酶水解的影响。以 Humicola insolens cutinase（HiC）作为 PET 织物水解的生物催化剂，研究了 DES 作为添加剂对提高酶水解 PET 织物产量的作用。结果表明，在酶浓度为 6.5% v/v（酶体积占总体积的比例）、温度为 60 °C、反应时间为 72 小时的条件下，低浓度（20% v/v）的 DES（甜菜碱：山梨醇；摩尔比为 1:2）可将水解产率提高 1.5 倍以上。在 DES 水溶液（甜菜碱：山梨醇；摩尔比为 1:2）和 DES 单组分水溶液（甜菜碱、山梨醇不合成 DES）中的酶水解表明，水解产率的增加主要是由于甜菜碱和山梨醇之间形成氢键，而不是单个组分的叠加。进一步分析表明，HiC 在低 DES 浓度下表现出较高的相对酶活性和稳定性。此外，CD 光谱和荧光光谱分析表明，DES 能有效保持 HiC 的结构。我们的工作为开发高效、可持续的方法来增强 PET 织物的 HiC 水解提供了见解，为在 PET 织物的生物改性中综合利用 DES 发掘了新的机遇和潜力。
期刊介绍：
The Journal of Polymers and the Environment fills the need for an international forum in this diverse and rapidly expanding field. The journal serves a crucial role for the publication of information from a wide range of disciplines and is a central outlet for the publication of high-quality peer-reviewed original papers, review articles and short communications. The journal is intentionally interdisciplinary in regard to contributions and covers the following subjects - polymers, environmentally degradable polymers, and degradation pathways: biological, photochemical, oxidative and hydrolytic; new environmental materials: derived by chemical and biosynthetic routes; environmental blends and composites; developments in processing and reactive processing of environmental polymers; characterization of environmental materials: mechanical, physical, thermal, rheological, morphological, and others; recyclable polymers and plastics recycling environmental testing: in-laboratory simulations, outdoor exposures, and standardization of methodologies; environmental fate: end products and intermediates of biodegradation; microbiology and enzymology of polymer biodegradation; solid-waste management and public legislation specific to environmental polymers; and other related topics.
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