微环境的微调以优化在多变体金属有机框架中固定的酶的催化活性
Yi-Ming Li1, Jian Yuan2, Hao Ren1
1School of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189, P. R. China.
Journal of the American Chemical Society
|September 3, 2021
概括
研究人员通过调整孔隙水友性来优化金属有机框架 (MOF) 中的酶活性. 这种策略提高了酶的稳定性和催化性能,证明了酶工程的新方法.
科学领域:
- 材料科学
- 生物化学
- 化学工程
背景情况:
- 通过人工工程增强酶活性是一个重大挑战.
- 金属有机框架 (MOFs),特别是热立体胺酸框架 (ZIFs),为封装和修改酶提供可调的平台.
- 非同位素的网状化学可以精确地控制MOF孔环境.
研究的目的:
- 在多变量ZIF-8 (MTV-ZIF-8) 框架内封装的BCL酶的活性.
- 通过孔隙微环境修改来调整框架-酶相互作用的策略.
- 调查链接器组成与酶性能之间的相关性.
主要方法:
- 使用多变量 (MTV) 方法来改变 ZIF-8 中的链接器功能和比率.
- 开发了组件调整三元图 (CAT) 方法进行系统分析.
- 采用FTIR光谱和光研究来确认酶形状的变化.
主要成果:
- 在MTV-ZIF-8中发现了酶BCL活性与水友性链接器比率之间的非线性相关性.
- 确定了影响酶构成的功能组的特定空间排列 (闭盖与开盖).
- 在优化BCL@ZIF-8的动态分辨率中,实现了加倍的催化反应率和99%的反体过量 (ee).
结论:
- 通过调整孔水友性,MTV方法提供了一种优化封装酶活性的方法.
- 在ZIF-8框架内,酶形状的变化对活性调节至关重要.
- 与自由酶相比,优化的BCL@ZIF-8具有更高的稳定性和催化效率.
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