Gizzie Evan A, LeBlanc Gabriel, Jennings G Kane, Cliffel David E
†Department of Chemistry, Vanderbilt University, Nashville, Tennessee 37235-1822, United States.
‡Department of Chemical and Biomolecular Engineering, Vanderbilt University, Nashville, Tennessee 37235-1604, United States.
ACS Appl Mater Interfaces. 2015 May 13;7(18):9328-35. doi: 10.1021/acsami.5b01065. Epub 2015 May 4.
In this work, we report for the first time the entrapment of the biomolecular supercomplex Photosystem I (PSI) within a conductive polymer network of polyaniline via electrochemical copolymerization. Composite polymer-protein films were prepared on gold electrodes through potentiostatic electropolymerization from a single aqueous solution containing both aniline and PSI. This study demonstrates the controllable integration of large membrane proteins into rapidly prepared composite films, the entrapment of such proteins was observed through photoelectrochemical analysis. PSI's unique function as a highly efficient biomolecular photodiode generated a significant enhancement in photocurrent generation for the PSI-loaded polyaniline films, compared to pristine polyaniline films, and dropcast PSI films. A comprehensive study was then performed to separately evaluate film thickness and PSI concentration in the initial polymerization solution and their effects on the net photocurrent of this novel material. The best performing composite films were prepared with 0.1 μM PSI in the polymerization solution and deposited to a film thickness of 185 nm, resulting in an average photocurrent density of 5.7 μA cm(-2) with an efficiency of 0.005%. This photocurrent output represents an enhancement greater than 2-fold over bare polyaniline films and 200-fold over a traditional PSI multilayer film of comparable thickness.
在本工作中,我们首次报道了通过电化学共聚将生物分子超复合物光系统I(PSI)包埋在聚苯胺导电聚合物网络中。通过恒电位电聚合,从含有苯胺和PSI的单一水溶液在金电极上制备复合聚合物-蛋白质膜。本研究证明了将大的膜蛋白可控地整合到快速制备的复合膜中,通过光电化学分析观察到了此类蛋白的包埋。与原始聚苯胺膜和滴铸PSI膜相比,PSI作为高效生物分子光电二极管的独特功能使得负载PSI的聚苯胺膜的光电流产生显著增强。然后进行了一项综合研究,以分别评估初始聚合溶液中的膜厚度和PSI浓度及其对这种新型材料净光电流的影响。在聚合溶液中使用0.1 μM PSI制备出性能最佳的复合膜,并将其沉积至185 nm的膜厚度,得到平均光电流密度为5.7 μA cm(-2),效率为0.005%。这种光电流输出比裸聚苯胺膜增强了2倍以上,比厚度相当的传统PSI多层膜增强了200倍以上。