生物衍生酸和酶催化水解降解ROMP热固性材料：从网状材料到线状材料
Hydrolytic degradation of ROMP thermosetting materials catalysed by bio-derived acids and enzyme: from network to linear materials
摘要：
本文报道了第一个由来自解纤维素热裂菌的生物衍生酸和角质酶（Thc_Cut1）催化的可降解ROMP热固性材料的实例。ROMP热固性材料是基于仅在交联部分中含有缩醛酯基团的异戊二烯二甲酰亚胺。使用生物衍生的乙酸和柠檬酸对不溶性交联材料进行酸催化水解，并使用Thc_Cut 1进行酶促降解，使材料完全溶于二氯甲烷。酸催化水解后的材料进行的1H NMR和流变学分析显示出与线性聚合物类似物不可区分的特征。这些分析证实了降解后交联部分的裂解，主链保持完整。酸催化水解后的聚合物材料的玻璃化转变温度与线性聚合物类似物所观察到的相同。TGA显示交联聚合物热稳定至150 °C，超过该温度显示由于缩醛酯键的热裂解而导致的重量损失。
英文摘要：
This paper reports the first example of the degradable ROMP thermosetting materials catalysed by bio-derived acids and cutinase from Thermobifida cellulosilytica (Thc_Cut1). The ROMP thermosetting materials are based on norbornene dicarboximides containing acetal ester groups only in the crosslink moiety. The insoluble cross-linked materials were subjected to acid-catalysed hydrolysis using bio-derived acetic and citric acids as well as enzymatic degradation using Thc_Cut1, resulting in the materials becoming completely soluble in dichloromethane. 1H NMR and rheological analysis performed on materials after acid-catalysed hydrolysis showed characteristics indistinguishable to that of the linear polymer analogues. These analyses confirmed the cleavage of the crosslink moiety upon degradation with the main backbone chains remaining intact. The glass transition temperatures of the polymer materials after acid-catalysed hydrolysis were the same of those observed for the linear polymer analogue. TGA showed that the cross-linked polymers thermally stable to 150 °C, beyond which showed weight losses due to the thermal cleavage of the acetal ester linkages.
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