介观结构二氧化硅-表面活性剂膜中功能活性蛋白视紫红质膜蛋白分子的共组装,Chemistry of Materials

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介观结构二氧化硅-表面活性剂膜中功能活性蛋白视紫红质膜蛋白分子的共组装
Chemistry of Materials ( IF 7.2 ) Pub Date : 2023-10-05 , DOI: 10.1021/acs.chemmater.3c01303
Maxwell W. Berkow ₁ , Hosu Gwak ₁ , Matthew N. Idso ₁ , Michael B. Schmithorst ₁ , Bailey E. Rhodes ₂ , Brad D. Price ₃ , Daniel S. Gianola ₂ , Songi Han _{1,

4} , Bradley F. Chmelka ₁

Affiliation

非离子、阳离子和两性离子表面活性剂的组合既可以稳定跨膜蛋白蛋白视紫红质，也可以直接共组装成坚固的透明介观结构二氧化硅-表面活性剂薄膜，其中含有高负载的功能活性蛋白客体。蛋白视紫红质是一种跨膜蛋白，具有光激活的 H ⁺传输特性，其光循环动力学可通过时间分辨紫外可见光谱进行量化，并且与天然脂质相比，与非生物介观结构膜中的蛋白视紫红质相似。表面活性剂介导关键离子通道残基的 pKa ，从而扩大了介观结构二氧化硅-表面活性剂主体材料中蛋白视紫红质的 pH 功能范围_。100 μm 薄膜的小角 X 射线衍射结果显示，蛋白质负载量高达 25 wt%，具有高度的介观尺度有序性，并且蛋白视紫红质具有 44 wt% 的蠕虫状介观结构有序性。固态¹ H、¹³ C 和²⁹ Si NMR 分析提供了对介孔通道表面的组成和相互作用的原子尺度见解，这解释了表面活性剂物种的结构导向作用。纳米压痕测量揭示了薄膜的机械稳健性，有趣的是，机械稳健性随着所检测的组合物的变形视紫红质负载而增加。热处理分析表明，在介观结构有序薄膜中，变形视紫红质的热稳定性提高至 110 °C。结果建立了二氧化硅-表面活性剂-蛋白视紫红质薄膜的成分、纳米和介观结构、光循环动力学以及宏观机械性能和热稳定性之间的密切相关关系，提供了关键的仿生设计标准。

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Co-Assembly of Functionally Active Proteorhodopsin Membrane Protein Molecules in Mesostructured Silica–Surfactant Films

A combination of nonionic, cationic, and zwitterionic surfactants is shown both to stabilize the transmembrane protein proteorhodopsin, as well as to direct coassembly into robust transparent mesostructured silica–surfactant films containing high loadings of functionally active protein guests. Proteorhodopsin is a transmembrane protein that exhibits light-activated H⁺ transport properties, the photocycle kinetics of which are quantified by time-resolved UV–visible spectroscopy and demonstrated to be similar to proteorhodopsin in the abiotic mesostructured films compared to native-like lipids. The surfactants mediate the pK_a of a key ion-channel residue, leading to an expanded pH functional range for proteorhodopsin in mesostructured silica–surfactant host materials. Small-angle X-ray diffraction results for 100-μm films show high extents of mesoscale order with protein loadings up to 25 wt % and wormlike mesostructural order for 44 wt % proteorhodopsin. Solid-state ¹H, ¹³C, and ²⁹Si NMR analyses provide atomic-scale insights into the compositions and interactions at the mesochannel surfaces, which account for the structure-directing roles of surfactant species. Nanoindentation measurements reveal the mechanical robustness of the films, which interestingly increases with proteorhodopsin loading for the compositions examined. Heat treatment analyses show improved thermal stability for proteorhodopsin to 110 °C within mesostructurally ordered films. The results establish closely correlated relationships between the compositions, nano- and mesoscale structures, photocycle kinetics, and macroscopic mechanical properties and thermal stabilities of the silica–surfactant- proteorhodopsin films, providing key biomimetic design criteria.

更新日期：2023-10-05

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