Department of Chemistry, Indian Institute of Technology (BHU), Varanasi, UP, 221005, India.
Department of Chemical & Environmental Engineering and Materials Science & Engineering Program, University of California-Riverside, Riverside, CA, 92521, USA.
Nat Commun. 2022 Mar 21;13(1):1505. doi: 10.1038/s41467-022-28942-0.
Enzymes are extremely complex catalytic structures with immense biological and technological importance. Nevertheless, their widespread environmental implementation faces several challenges, including high production costs, low operational stability, and intricate recovery and reusability. Therefore, the de novo design of minimalistic biomolecular nanomaterials that can efficiently mimic the biocatalytic function (bionanozymes) and overcome the limitations of natural enzymes is a critical goal in biomolecular engineering. Here, we report an exceptionally simple yet highly active and robust single amino acid bionanozyme that can catalyze the rapid oxidation of environmentally toxic phenolic contaminates and serves as an ultrasensitive tool to detect biologically important neurotransmitters similar to the laccase enzyme. While inspired by the laccase catalytic site, the substantially simpler copper-coordinated bionanozyme is ∼5400 times more cost-effective, four orders more efficient, and 36 times more sensitive compared to the natural protein. Furthermore, the designed mimic is stable under extreme conditions (pH, ionic strength, temperature, storage time), markedly reusable for several cycles, and displays broad substrate specificity. These findings hold great promise in developing efficient bionanozymes for analytical chemistry, environmental protection, and biotechnology.
酶是具有巨大生物学和技术重要性的极其复杂的催化结构。然而,它们在广泛的环境应用中面临着一些挑战,包括高生产成本、低操作稳定性以及复杂的回收和再利用。因此,从头设计能够高效模拟生物催化功能的极简生物分子纳米材料(仿生酶),克服天然酶的局限性,是生物分子工程的一个关键目标。在这里,我们报告了一种非常简单但高度活跃和稳健的单一氨基酸仿生酶,它可以催化环境有毒酚类污染物的快速氧化,并作为一种超灵敏的工具来检测类似于漆酶的生物重要神经递质。虽然仿生酶的设计灵感来自漆酶的催化位点,但与天然蛋白质相比,这种结构大大简化的铜配位仿生酶的成本效益高 5400 倍,效率高 4 个数量级,灵敏度高 36 倍。此外,设计的模拟酶在极端条件(pH 值、离子强度、温度、储存时间)下稳定,可显著重复使用多个循环,并具有广泛的底物特异性。这些发现为分析化学、环境保护和生物技术领域开发高效仿生酶提供了很大的希望。