Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
School of Mechanical Engineering, Purdue University, Birck Nanotechnology Center, Bindley Bioscience Center, West Lafayette, Indiana 47907, USA.
Nat Chem. 2010 Nov;2(11):929-936. doi: 10.1038/nchem.822. Epub 2010 Sep 5.
Naturally occurring photosynthetic systems use elaborate pathways of self-repair to limit the impact of photo-damage. Here, we demonstrate a complex consisting of two recombinant proteins, phospholipids and a carbon nanotube that mimics this process. The components self-assemble into a configuration in which an array of lipid bilayers aggregate on the surface of the carbon nanotube, creating a platform for the attachment of light-converting proteins. The system can disassemble upon the addition of a surfactant and reassemble upon its removal over an indefinite number of cycles. The assembly is thermodynamically metastable and can only transition reversibly if the rate of surfactant removal exceeds a threshold value. Only in the assembled state do the complexes exhibit photoelectrochemical activity. We demonstrate a regeneration cycle that uses surfactant to switch between assembled and disassembled states, resulting in an increased photoconversion efficiency of more than 300% over 168 hours and an indefinite extension of the system lifetime.
天然存在的光合作用系统利用精细的自我修复途径来限制光损伤的影响。在这里，我们展示了一种由两种重组蛋白、磷脂和碳纳米管组成的复合物，该复合物模拟了这一过程。这些组件自行组装成一种结构，其中脂质双层的阵列在碳纳米管的表面聚集，为光转化蛋白的附着创造了一个平台。该系统可以在添加表面活性剂时解组装，并在其去除后在无限数量的循环中重新组装。该组装是热力学亚稳态的，只有在表面活性剂去除速率超过阈值时才能可逆地转变。只有在组装状态下，复合物才表现出光电化学活性。我们展示了一个再生循环，该循环使用表面活性剂在组装和去组装状态之间切换，导致在 168 小时内光转化率提高了 300%以上，并且系统寿命无限延长。
