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Stationary photocurrent generation from bacteriorhodopsin-loaded lipo-polymersomes in polyelectrolyte multilayer assembly on polyethersulfone membrane.
Analytical and Bioanalytical Chemistry ( IF 4.3 ) Pub Date : 2020-03-12 , DOI: 10.1007/s00216-020-02533-8
Agnieszka Mech-Dorosz 1, 2 , Niada Bajraktari 3, 4 , Claus Hélix-Nielsen 3, 4 , Jenny Emnéus 1 , Arto Heiskanen 1
Affiliation  

Abstract

Vesicles constructed of either synthetic polymers alone (polymersomes) or a combination of polymers and lipids (lipo-polymersomes) demonstrate excellent long-term stability and ability to integrate membrane proteins. Applications using lipo-polymersomes with integrated membrane proteins require suitable supports to maintain protein functionality. Using lipo-polymersomes loaded with the light-driven proton pump bacteriorhodopsin (BR), we demonstrate here how the photocurrent is influenced by a chosen support. In our study, we deposited BR-loaded lipo-polymersomes in a cross-linked polyelectrolyte multilayer assembly either directly physisorbed on gold electrode microchips or cross-linked on an intermediary polyethersulfone (PES) membrane covalently grafted using a hydrogel cushion. In both cases, electrochemical impedance spectroscopic characterization demonstrated successful polyelectrolyte assembly with BR-loaded lipo-polymersomes. Light-induced proton pumping by BR-loaded lipo-polymersomes in the different support constructs was characterized by amperometric recording of the generated photocurrent. Application of the hydrogel/PES membrane support together with the polyelectrolyte assembly decreased the transient current response upon light activation of BR, while enhancing the generated stationary current to over 700 nA/cm2. On the other hand, the current response from BR-loaded lipo-polymersomes in a polyelectrolyte assembly without the hydrogel/PES membrane support was primarily a transient peak combined with a low-nanoampere-level stationary photocurrent. Hence, the obtained results demonstrated that by using a hydrogel/PES support it was feasible to monitor continuously light-induced proton flux in biomimetic applications of lipo-polymersomes.

Graphical abstract



中文翻译:

在聚醚砜膜上的聚电解质多层组件中,由载有细菌视紫红质的脂质聚合物体产生固定光电流。

摘要

由单独的合成聚合物(聚合物囊泡)或聚合物和脂质的组合(脂质聚合物囊泡)构成的囊泡表现出优异的长期稳定性和整合膜蛋白的能力。使用具有集成膜蛋白的脂质聚合物体的应用需要合适的支持来维持蛋白质功能。使用装载有光驱动质子泵细菌视紫红质 (BR) 的脂质聚合物体,我们在这里演示了光电流如何受到所选支持的影响。在我们的研究中,我们将载有 BR 的脂质聚合物体沉积在交联聚电解质多层组件中,该组件直接物理吸附在金电极微芯片上,或者交联在使用水凝胶垫共价接枝的中间聚醚砜 (PES) 膜上。在这两种情况下,电化学阻抗光谱表征证明聚电解质与负载 BR 的脂质聚合物体成功组装。不同载体结构中负载 BR 的脂质聚合物体的光诱导质子泵浦的特征在于产生的光电流的安培记录。水凝胶/PES 膜支撑与聚电解质组件的应用降低了 BR 光激活时的瞬态电流响应,同时将产生的固定电流提高到 700 nA/cm 以上2 . 另一方面,在没有水凝胶/PES 膜支撑的聚电解质组件中,负载 BR 的脂质聚合物体的电流响应主要是一个瞬态峰,结合了低纳安级的固定光电流。因此,获得的结果表明,通过使用水凝胶/PES 支持,在脂质聚合物体的仿生应用中连续监测光诱导的质子通量是可行的。

更新日期:2020-03-12
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