Tyrosinase-functionalized polyhydroxyalkanoate bio-beads as a novel biocatalyst for degradation of bisphenol analogues
Tyrosinase-functionalized polyhydroxyalkanoate bio-beads as a novel biocatalyst for degradation of bisphenol analogues
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DOI：
10.1016/j.envint.2022.107225
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发表时间：
2022-04-07
影响因子：
11.8
通讯作者：
Wei，Na
中科院分区：
文献类型：
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作者：
Zhu，Baotong;Wei，Na
双酚化合物是一种新兴的污染物，具有已知的内分泌干扰作用。生物催化为水回收的深度处理提供了一种绿色化学替代方法。本研究利用合成生物学技术，将巨巨酪氨酸芽孢杆菌（bacillus megaterumtyrosinase, BmTyr）基因固定在自组装聚羟基烷酸酯（PHA）生物聚合物微球（PHA -BmTyr）表面，创造了一种新型生物催化剂，并首次在体内证明了该生物催化剂的一锅式生产，可有效降解和解毒各种双酚类似物。双酚类物质的降解途径由BmTyr的单酚酶和二酚酶活性介导。值得注意的是，PHA-BmTyr生物催化双酚降解可以显著降低或消除污染物的雌激素活性，降解产物的急性和慢性毒性明显低于其母体化合物。此外，PHA-BmTyr生物催化剂在多次双酚降解反应循环中具有很高的可重复使用性，并且在4℃和室温下分别保存30 d时，其稳定性良好，保持了100%和86.6%的初始活性。此外，PHA-BmTyr生物催化剂可有效降解实际废水出水基质中的双酚类似物。该研究为开发可持续水回收的创新生物催化技术提供了一条有希望的途径。
Bisphenol compounds are emerging contaminants of high concerns with known endocrine-disrupting effects. Biocatalysis provides a green chemistry alternative for advanced treatment in water reclamation. This study created a novel biocatalyst through genetically immobilizing theBacillus megateriumtyrosinase enzyme (BmTyr) on the surface of self-assembled polyhydroxyalkanoate (PHA) biopolymer beads (termed PHA-BmTyr) by using synthetic biology techniques and demonstrated one-pot in vivo production of the biocatalyst for effective degradation and detoxification of various bisphenol analogues for the first time. The degradation pathway of bisphenols was determined to be mediated by the monophenolase and diphenolase activity of BmTyr. Notably, biocatalytic bisphenol degradation by PHA-BmTyr could substantially reduce or eliminate estrogenic activity of the contaminants, and the degradation products had remarkably lower acute and chronic toxicity than their parent compounds. Furthermore, the PHA-BmTyr biocatalyst had high reusability for multiple bisphenol degradation reaction cycles and showed excellent stability that retained 100% and 86.6% of the initial activity when stored at 4 °C and room temperature, respectively for 30 days. Also, the PHA-BmTyr biocatalyst could efficiently degrade bisphenol analogues in real wastewater effluent matrix. This study provides a promising approach to develop innovative biocatalysis technologies for sustainable water reclamation.