Degradation Behavior of Aliphatic–Aromatic Polyesters: from Microplastic-free Composting to Enzyme-Driven Recycling Possibility

IF 4.4 2区 化学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Ashank Upadhyay, Onur Turak, Emilia Fulajtar, Christopher R. Greve, Eva M. Herzig, Birte Höcker and Seema Agarwal*, 
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引用次数: 0

Abstract

To develop a polymer that leaves no microplastic traces in compost and is recyclable, this study investigates the degradation behavior of custom-designed synthetic aliphatic–aromatic polyesters. These polyesters, synthesized via melt polycondensation from 1,4-benzenedimethanol and aliphatic diacids of varying chain lengths, underwent comprehensive degradation experiments in alkaline solutions, industrial compost, sludge water, and with five enzymes: commercially obtained Hi-Cutinase (HiC), Esterase EL-01, and in-house-produced Ideonella sakaiensis PETase (IsPETase), Cryptosporangium aurantiacum PETase variant M9(CaPETase), and metagenomic leaf-branch compost cutinase variant ICCG (LCCICCG). The degradation behavior was correlated with polymer properties, including chemical structure, melting point, hydrophobicity, and crystallinity. Spiking and compost extraction experiments confirmed complete degradation of all polyesters under study within 12 weeks in industrial compost, leaving no detectable plastic residues. Enzymatic studies identified HiC as the most effective enzyme for these polyesters at 30 °C, while odd-carbon-containing polyesters served as good substrates for Esterase EL-01, HiC, and IsPETase. In contrast, aromatic PET, even with low crystallinity, showed no enzymatic specificity with these enzymes.

Abstract Image

脂肪族-芳香族聚酯的降解行为:从无微塑料堆肥到酶驱动回收的可能性
为了开发一种不会在堆肥中留下微塑料痕迹且可回收的聚合物,本研究调查了定制合成脂肪族芳香族聚酯的降解行为。这些聚酯由不同链长的1,4-苯二甲醇和脂肪二酸通过熔融缩聚合成,并在碱性溶液、工业堆肥、污泥水和五种酶中进行了全面的降解实验:商业获得的高角质酶(HiC),酯酶EL-01,和内部生产的酒井Ideonella sakaiensis PETase (IsPETase),金隐孢子菌PETase变体M9(CaPETase),以及宏基因组叶枝堆肥角质酶变体ICCG (LCCICCG)。降解行为与聚合物的性质有关,包括化学结构、熔点、疏水性和结晶度。钉钉和堆肥提取实验证实,在工业堆肥中,所有聚酯在12周内完全降解,没有留下可检测到的塑料残留物。酶学研究发现,在30°C时,HiC是对这些聚酯最有效的酶,而奇数碳含聚酯是酯酶EL-01、HiC和IsPETase的良好底物。相比之下,芳香PET即使结晶度低,对这些酶也没有特异性。
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来源期刊
CiteScore
7.20
自引率
6.00%
发文量
810
期刊介绍: ACS Applied Polymer Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics, and biology relevant to applications of polymers. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrates fundamental knowledge in the areas of materials, engineering, physics, bioscience, polymer science and chemistry into important polymer applications. The journal is specifically interested in work that addresses relationships among structure, processing, morphology, chemistry, properties, and function as well as work that provide insights into mechanisms critical to the performance of the polymer for applications.
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