叶绿素/ TiO <sub>2</sub> /脂质共组装模拟类囊体膜的集光与除氧,ACS Applied Materials & Interfaces

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叶绿素/ TiO ₂ /脂质共组装模拟类囊体膜的集光与除氧
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-02-26 , DOI: 10.1021/acsami.0c21662
Shukun Shen _{1,

2} , Yiyun Wang ₁ , Jingxuan Dong ₁ , Rui Zhang ₁ , Atul Parikh ₃ , Jian-Gang Chen ₂ , Daodao Hu _{1,

2}

Affiliation

对于用于太阳能利用和转化的人造光合材料的设计和建造，人们越来越感兴趣。受类囊体膜结构的启发，我们在这里介绍了一种用于光收集和氧气释放的杂合结构。我们的设计在天然膜环境中将叶绿素与TiO ₂共轭。利用脂质的天然双层结构来定位两亲叶绿素a水合过程中脂质体膜中的疏水性钛酸四丁酯TBOT。该共组装结构模仿类囊体膜的基本结构，其特征在于结合了场发射扫描电子显微镜（SEM），透射电子显微镜（TEM），能量色散X射线光谱仪（EDS），拉曼光谱，压力（π）-面积（A）等温线，循环伏安法（CV）和电化学阻抗谱（EIS）分析。我们的结果证明叶绿素a成功插入膜中并证实了TiO _2的原位形成纳米壳被限制在脂质双层/水界面。我们进一步表明，杂化脂质体在可见光收集和氧气释放中表现出明确的光活性，这很可能是由于TiO ₂壳的较大比表面积，叶绿素分子与TiO ₂薄层的有效界面结合所致。密度泛函理论（DFT）的计算符合电子注入过程。我们希望目前的工作将为集光颜料之间的界面复合及其敏化光催化开辟新的见解，并开发一种新型的人造光合材料零成本的环境退化和高效率的光催化O ₂ 生产。

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Mimicking Thylakoid Membrane with Chlorophyll/TiO2/Lipid Co-Assembly for Light-Harvesting and Oxygen Releasing

There is a growing interest in the design and construction of artificial photosythetic materials for solar energy utilization and conversion. Inspired by the structure of thylakoid membrane, we present here a hybrid construct for light-harvesting and oxygen releasing. Our design conjugates chlorophyll to TiO₂ in a native-like membrane environment. The natural bilayer structure of lipids is utilized to localize the amphiphilic chlorophyll a and hydrophobic tetrabutyl titanate TBOT in the liposomal membrane during hydration process. The coassembled structure, which mimics the essential organization of the thylakoid membrane, is characterized using a combination of field emission scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive X-ray spectrometer (EDS), Ramam spectra, pressure (π)-area (Α) isotherms, cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS) analysis. Our results demonstrate successful insertation of chlorophyll a in the membrane and confirm the in situ formation of TiO₂ nanoshell confined at the lipid bilayer/water interface. We further show that the hybrid liposomes exhibit unambiguous photoactivity in visible light-harvesting and oxygen release, likely resulting from a larger specific surface area of the TiO₂ shell, an efficient interfacial conjugation of the chlorophyll molecules with the thin TiO₂ layer. The density functional theory (DFT) calculations were in accordance with the eletron injection processes.We expect that the present work will open a new insight into interfacial recombination between light-harvesting pigments and their sensitized photocatalysis, and develop a new kind of artificial photosynthetic materials with zero-cost of environmental degradation and high efficiency for the photocatalytic O₂ production.

更新日期：2021-03-10

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