Leiden Institute of Chemistry, Leiden University, Einsteinweg 55, Leiden, 2333 CC, The Netherlands.
Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, UK.
Chem Soc Rev. 2021 Apr 26;50(8):4833-4855. doi: 10.1039/d0cs00737d.
Artificial photosynthesis has experienced rapid developments aimed at producing photocatalytic systems for the synthesis of chemical energy carriers. Conceptual advances of solar fuel systems have been inspired by improved understanding of natural photosynthesis and its key operational principles: (a) light harvesting, (b) charge separation, (c) directional proton and electron transport between reaction centres and across membranes, (d) water oxidation and (e) proton or CO2 reduction catalysis. Recently, there has been a surge of bio-inspired photosynthetic assemblies that use liposomes as nanocompartments to confine reaction spaces and enable vectorial charge transport across membranes. This approach, already investigated in the 1980s, offers in principle a promising platform for solar fuel synthesis. However, the fundamental principles governing the supramolecular assemblies of lipids and photoactive surfactant-like molecules in membranes, are intricate, and mastering membrane-supported photochemistry requires thorough understanding of the science behind liposomes. In this review, we provide an overview of approaches and considerations to construct a (semi)artificial liposome for solar fuel production. Key features to consider for the use of liposomes in solar fuel synthesis are highlighted, including the understanding of the orientation and binding of different components along the membrane, the controlled electron transport between the reaction centres, and the generation of proton gradients as driving force. Together with a list of experimental techniques for the characterisation of photoactive liposomes, this article provides the reader with a roadmap towards photocatalytic fuel production at the interface of lipid membranes and aqueous media.
人工光合作用经历了快速的发展，旨在为化学能量载体的合成生产光催化系统。受对自然光合作用及其关键操作原理（a）光捕获、（b）电荷分离、（c）反应中心之间和跨膜的定向质子和电子传输、（d）水氧化和（e）质子或 CO2还原催化的深入理解的启发，太阳能燃料系统的概念取得了进步。最近，涌现出了许多受生物启发的光合组装体，它们使用脂质体作为纳米隔室来限制反应空间，并实现跨膜的定向电荷传输。这种方法在 20 世纪 80 年代已经进行了研究，原则上为太阳能燃料合成提供了一个很有前途的平台。然而，控制脂质和类光活性表面活性剂分子在膜中超分子组装的基本原理错综复杂，要掌握膜支撑的光化学，需要深入了解脂质体背后的科学。在这篇综述中，我们概述了构建（半）人工脂质体用于太阳能燃料生产的方法和考虑因素。突出了在太阳能燃料合成中使用脂质体时需要考虑的关键特征，包括理解不同组件在膜中的取向和结合、反应中心之间的受控电子传输以及质子梯度的产生作为驱动力。本文结合了一系列用于光活性脂质体表征的实验技术，为在脂质膜和水相界面处进行光催化燃料生产提供了路线图。
