Molecular insights into the catalytic mechanism of plasticizer degradation by a monoalkyl phthalate hydrolase.

Molecular insights into the catalytic mechanism of plasticizer degradation by a monoalkyl phthalate hydrolase.
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DOI:
10.1038/s42004-023-00846-0
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发表时间:
2023-03-01
影响因子:
5.9
通讯作者:
Wang, Yonghua
Wang, Yonghua
中科院分区:
化学2区
文献类型:
--
作者:
Chen, Yebao;Wang, Yongjin;Xu, Yang;Sun, Jiaojiao;Yang, Liu;Feng, Chenhao;Wang, Jia;Zhou, Yang;Zhang, Zhi-Min;Wang, Yonghua

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邻苯二甲酸酯(PAEs)是一类被广泛用作增塑剂的外来化合物,因其对人类健康和环境的不良影响而受到越来越多的关注。利用PAE水解酶进行微生物降解是一种很有前途的处理方法。然而,到目前为止,只有有限数量的PAE水解酶被表征。在这里,我们报道了MehpH的结构,它是一种邻苯二甲酸单烷基(MBP)水解酶,催化MBP反应生成邻苯二甲酸和相应的醇,以apo和配体结合的形式存在。这些结构显示了一个带正电的催化中心,与MBP上带负电的羧基互补,以及一个作为酒精出口的穿透隧道。这项研究首次揭示了PAE水解酶的酶-底物结合模型,为未来开发更好的酶提供了有力的支持。邻苯二甲酸酯水解酶在微生物降解邻苯二甲酸酯增塑剂方面具有广阔的应用前景,但目前仅有少量PAE水解酶被表征。在这里,作者报道了MehpH的结构和功能特征,MehpH是一种将邻苯二甲酸单烷基酯(MBP)降解为邻苯二甲酸和丁醇的水解酶。
Phthalate acid esters (PAEs), a group of xenobiotic compounds used extensively as plasticizers, have attracted increasing concern for adverse effects to human health and the environment. Microbial degradation relying on PAE hydrolases is a promising treatment. However, only a limited number of PAE hydrolases were characterized to date. Here we report the structures of MehpH, a monoalkyl phthalate (MBP) hydrolase that catalyzes the reaction of MBP to phthalic acid and the corresponding alcohol, in apo and ligand-bound form. The structures reveal a positively-charged catalytic center, complementary to the negatively-charged carboxyl group on MBP, and a penetrating tunnel that serves as exit of alcohol. The study provides a first glimpse into the enzyme-substrate binding model for PAE hydrolases, leading strong support to the development of better enzymes in the future. Phthalate acid ester hydrolases are of promise for the microbial degradation of phthalate acid ester plasticizers, however, only a small number of PAE hydrolases have been characterized. Here, the authors report the structural and functional characterization of MehpH, a monoalkyl phthalate (MBP) hydrolase that degrades MBP to phthalic acid and butanol.
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