Hydrolase-Catalyzed Depolymerization Mechanism toward Crystalline and Amorphous Polyethylene Terephthalate

被引:1
作者
Zheng, Mingna [1 ]
Li, Yanwei [1 ]
Dong, Weiliang [2 ]
Zhang, Qingzhu [1 ]
Wang, Wenxing [1 ]
机构
[1] Shandong Univ, Environm Res Inst, Qingdao 266237, Peoples R China
[2] Nanjing Tech Univ, Coll Biotechnol & Pharmaceut Engn, Nanjing 211800, Peoples R China
来源
ACS SUSTAINABLE CHEMISTRY & ENGINEERING | 2024年 / 12卷 / 27期
基金
中国国家自然科学基金;
关键词
polyethylene terephthalate; biodepolymerization; crystalline region; conformational selection; enzymeengineering; DISTORTION-INTERACTION ANALYSIS; POLY(ETHYLENE-TEREPHTHALATE); DEGRADATION; REACTIVITY; PLASTICS; DESIGN; CHARMM;
D O I
10.1021/acssuschemeng.4c02986
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Enzyme-based recycling of the extensively utilized polyethylene terephthalate (PET) is considered as a promising eco-friendly strategy to manage PET waste. Although efficient depolymerization of amorphous PET has been achieved, highly efficient depolymerization of the well-ordered crystalline region of PET presents a huge challenge. Herein, leveraged to molecular dynamics simulations and quantum mechanics/molecular mechanics calculations, we study the depolymerization mechanism of IsPETase toward both crystalline and amorphous PET to unravel the origin of the efficient depolymerization of the amorphous region. We demonstrated that crystalline PET is not well accommodated within the active pocket, and significant distortion energy is needed during its depolymerization. Poor stabilization within the oxyanion hole for crystalline PET was identified and confirmed to lead to higher energy barriers. In addition, after identifying the rate-determining step, we reveal that IsPETase prefers to depolymerize trans than gauche conformation of the PET polymer with a 2.4 kcal mol(-1) lower energy barrier. Differences in structural/charge distributions within the active site of the enzyme between trans and gauche conformations were proposed to be responsible for this preference. The structure-charge-activity relationship for the rate-determining step was built. Our results will aid the rational engineering of PETases with high depolymerization efficiency toward the crystalline region of PET for fighting the challenges of industrial applications.
引用
收藏
页码:10252 / 10259
页数:8
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