Biomimetic Strategy To Reversibly Trigger Functionality of Catalytic Nanocompartments by the Insertion of pH-Responsive Biovalves
Biomimetic Strategy To Reversibly Trigger Functionality of Catalytic Nanocompartments by the Insertion of pH-Responsive Biovalves
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DOI：
10.1021/acs.nanolett.7b02886
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发表时间：
2017-09-01
期刊：
影响因子：
10.8
通讯作者：
Palivan, Cornelia G.
中科院分区：
文献类型：
--
作者：
Edlinger, Christoph;Einfalt, Tomaz;Palivan, Cornelia G.
我们描述了一种创新的策略，通过结合pH可逆的生物阀和酶负载的合成室，在纳米级水平上产生具有触发功能的催化室。生物瓣膜已经通过将刺激响应肽附着到遗传修饰的通道孔蛋白而被工程化，从而使得能够响应于局部环境中的pH变化而可逆地改变通过孔蛋白的孔的分子流。生物阀功能性通过基于膜的渗透性的可逆变化来开启/关闭酶的原位活性，从而触发装载酶的隔室的腔内的反应，所述膜的渗透性的可逆变化阻断或允许底物和产物通过。我们的催化隔室的复杂功能是基于保持隔室的完整性以保护包封的酶。与游离酶相比，原位活性增加，并且在存在特定刺激时实现活性的可逆开/关开关。这种策略为开发催化纳米室提供了直接的解决方案，这些纳米室以受控的刺激响应方式有效地生产所需的分子，在医学，分析化学和催化等领域具有很高的潜力。
We describe an innovative strategy to generate catalytic compartments with triggered functionality at the nanoscale level by combining pH-reversible biovalves and enzyme-loaded synthetic compartments. The biovalve has been engineered by the attachment of stimuli responsive peptides to a genetically modified channel porin, enabling a reversible change of the molecular flow through the pores of the porin in response to a pH change in the local environment. The biovalve functionality triggers the reaction inside the cavity of the enzyme-loaded compartments by switching the in situ activity of the enzymes on/off based on a reversible change of the permeability of the membrane, which blocks or allows the passage of substrates and products. The complex functionality of our catalytic compartments is based on the preservation of the integrity of the compartments to protect encapsulated enzymes. An increase of the in situ activity compared to that of the free enzyme and a reversible on/off switch of the activity upon the presence of a specific stimulus is achieved. This strategy provides straightforward solutions for the development of catalytic nanocompartments efficiently producing desired molecules in a controlled, stimuli-responsive manner with high potential in areas, such as medicine, analytical chemistry, and catalysis.