Dynamic Docking-Assisted Engineering of Hydrolases for Efficient PET Depolymerization

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-02-21 DOI:10.1021/acscatal.4c00400

Yi Zheng, Qingbin Li, Pan Liu, Yingbo Yuan, Longyang Dian, Qian Wang, Quanfeng Liang, Tianyuan Su* and Qingsheng Qi*,

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Abstract

Poly(ethylene terephthalate) (PET) is the most abundant polyester plastic and is causing serious environmental pollution. Rapid biological depolymerization of PET waste at a large scale requires powerful engineered enzymes with excellent performance. Here, we designed a computational strategy to analyze the ligand affinity energy of enzymes to PET chains by molecular docking with the dynamic protein conformations, named affinity analysis based on dynamic docking (ADD). After three rounds of protein engineering assisted by ADD, we drastically enhanced the PET-depolymerizing activity of leaf-branch-compost cutinase (LCC). The best variant LCC-A2 depolymerized >90% of the pretreated, postconsumer PET waste into corresponding monomers within 3.3 h at 78 °C, and over 99% of the products was terminal depolymerization products (terephthalic acid and ethylene glycol), representing the fastest PET depolymerization rate reported to date in the bioreactor under optimal condition. Structural analysis revealed interesting features that improved the ligand affinity and catalytic performance. In conclusion, the proposed strategy and engineered variants represent a substantial advancement of the biological circular economy for PET.

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动态对接辅助水解酶工程，实现 PET 的高效解聚

聚对苯二甲酸乙二醇酯（PET）是最丰富的聚酯塑料，正在造成严重的环境污染。对 PET 废料进行大规模快速生物解聚需要性能卓越的强力工程酶。在此，我们设计了一种计算策略，通过与动态蛋白质构象的分子对接来分析酶与 PET 链的配体亲和能，命名为基于动态对接的亲和分析（ADD）。在 ADD 的辅助下，经过三轮蛋白质工程，我们大幅提高了叶枝-堆肥切蛋白酶（LCC）的 PET 解聚活性。最佳变体 LCC-A2 在 78 ℃、3.3 h 内将 90% 经过预处理的消费后 PET 废料解聚成相应的单体，超过 99% 的产物是终端解聚产物（对苯二甲酸和乙二醇），这是迄今为止在生物反应器中最佳条件下报道的最快 PET 解聚速度。结构分析揭示了提高配体亲和力和催化性能的有趣特征。总之，所提出的策略和工程变体代表了 PET 生物循环经济的巨大进步。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.