Supramolecular assembly of biohybrid photoconversion systems
Supramolecular assembly of biohybrid photoconversion systems
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DOI：
10.1039/c0ee00369g
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发表时间：
2011-01-01
影响因子：
32.5
通讯作者：
O'Neill, Hugh
中科院分区：
文献类型：
--
作者：
Cardoso, Mateus B.;Smolensky, Dmitriy;O'Neill, Hugh
自组装膜结构在开发将太阳能转化为电能或燃料的材料方面具有巨大的潜力。发现自然光合系统中促进自组装的设计原理可能会为合成太阳能转换系统的开发提供灵感。我们报告的第一次，自然发生的光捕获天线可以改变相行为的聚（环氧乙烷）-嵌段-聚（环氧丙烷）-嵌段-聚（环氧乙烷）（PEO-PPO-PEO）嵌段共聚物系统从胶束到层状结构模仿他们的作用，在维持超分子结构的光合膜。小角中子散射表明，PEO 43-PPO 16-PEO 43胶束经历了从胶束状态到层状结构的相变，在植物捕光复合物II（LHCII）的存在下，具有类似于60埃的空间重复。此外，分光光度分析表明，蛋白质自组装在合成膜结构。嵌段共聚物中嵌入的LHCII介导的光依赖性产氢的最大速率为6.4 mmol h（-1）/mg叶绿素。H-2的生产持续超过100小时，显示了这种方法用于开发自组装生物启发光转换系统的潜力。虽然激发能量转移是LHCII的主要功能，但这项工作提供了证据，表明蛋白质复合物也可以进行电子转移，这是一种在体内不知道发生的作用。这项工作的意义在于，它提供了一种新的方法，用于开发一类新的基于膜的智能材料，该材料具有依赖于相互作用组件的组装的良好控制的结构，并且它也可能在光转换器件中的能量转移的自修复和控制中具有重要意义。
Self-assembled membrane architectures have great potential for the development of materials for the conversion of solar energy into electricity or fuels. Discovering the design principles that promote self-assembly in natural photosynthetic systems may provide inspiration for the development of synthetic solar conversion systems. We report for the first time that naturally occurring light harvesting antennae can alter the phase behavior of a poly(ethylene oxide)-block-poly(propylene oxide)-block-poly(ethylene oxide) (PEO-PPO-PEO) block copolymer system from micellar to lamellar structures mimicking their role in maintaining the supramolecular architecture of the photosynthetic membrane. Small-angle neutron scattering shows that PEO43-PPO16-PEO43 micelles undergo a phase transition from a micellar state to a lamellar structure with a similar to 60 angstrom spatial repetition in the presence of plant light harvesting complex II (LHCII). In addition, spectrophotometric analysis indicates that the protein self-assembles in the synthetic membrane structure. Photodependent hydrogen production mediated by LHCII embedded in the block copolymer had a maximum rate of 6.4 mmol h(-1) per mg chlorophyll. The production of H-2 was sustained for greater than 100 hours showing the potential of this approach for the development of self-assembled bioinspired photoconversion systems. Although excited energy transfer is the primary function of LHCII, this work provides evidence that the protein complex can also perform electron transfer, a role not known to occur in vivo. The significance of this work is that it provides a novel approach for developing a new class of membrane-based smart material with a well-controlled architecture that is dependent on the assembly of interacting components, and it could also have important implications in self-repair and control of energy transfer in photoconversion devices.