Sun Yuting, Guo Ming, Hu Shengnan, Jia Yankun, Zhu Wenkai, Yamauchi Yusuke, Wang Chaohai
College of Environmental and Resource Sciences, Zhejiang Agricultural & Forestry University Hangzhou Zhejiang 311300 China.
College of Chemistry and Materials Engineering, Zhejiang Agricultural & Forestry University Hangzhou Zhejiang 311300 China
Chem Sci. 2024 Sep 18;15(42):17608-17. doi: 10.1039/d4sc03752a.
We present a study on an immobilized functional enzyme (IFE), a novel biomaterial with exceptional sustainability in enzyme utility, widely employed across various fields worldwide. However, conventional carriers are prone to eroding the active functional domain of the IFE, thereby weakening its intrinsic enzyme activity. Consequently, there is a burgeoning interest in developing next-generation IFEs. In this study, we engineered a carbon-based bifunctional heterogeneous enzyme (MIP-AMWCNTs@lipase) for the intelligent recognition of di(2-ethylhexyl)phthalate (DEHP), a common plasticizer. The heterogeneous enzyme contains a bifunctional structural domain that both enriches and degrades DEHP. We investigated its dual-response performance for the enrichment and specific removal of DEHP. The imprinting factor of the carrier for DEHP was 3.4, demonstrating selectivity for DEHP. The removal rate reached up to 94.2% over a short period. The heterogeneous enzyme exhibited robust activity, catalytic efficiency, and excellent stability under harsh environmental conditions, retaining 77.7% of its initial lipase activity after 7 cycles. Furthermore, we proposed a stepwise heterogeneous enzyme reaction kinetic model based on the Michaelis-Menten equation to enhance our understanding of enzyme reaction kinetics. Our study employs a dual-effect recognition strategy of molecular blotting and enzyme immobilization to establish a method for the removal of organic pollutants. These findings hold significant implications for the fields of biomaterials and environmental science.
我们展示了一项关于固定化功能酶（IFE）的研究，IFE是一种新型生物材料，在酶的应用中具有卓越的可持续性，在全球各个领域广泛使用。然而，传统载体容易侵蚀IFE的活性功能域，从而削弱其固有的酶活性。因此，人们对开发下一代IFE的兴趣日益浓厚。在本研究中，我们设计了一种基于碳的双功能异质酶（MIP-AMWCNTs@脂肪酶），用于智能识别常见增塑剂邻苯二甲酸二（2-乙基己基）酯（DEHP）。这种异质酶包含一个双功能结构域，既能富集又能降解DEHP。我们研究了其对DEHP的富集和特异性去除的双重响应性能。载体对DEHP的印迹因子为3.4，表明对DEHP具有选择性。在短时间内去除率高达94.2%。该异质酶在恶劣环境条件下表现出强大的活性、催化效率和出色的稳定性，7个循环后仍保留其初始脂肪酶活性的77.7%。此外，我们基于米氏方程提出了一种逐步异质酶反应动力学模型，以加深我们对酶反应动力学的理解。我们的研究采用分子印迹和酶固定化的双效识别策略，建立了一种去除有机污染物的方法。这些发现对生物材料和环境科学领域具有重要意义。
