Wang Lili, Wen Qi, Jia Pan, Jia Meijuan, Lu Diannan, Sun Xiaoming, Jiang Lei, Guo Wei
College of Science, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
CAS Key Laboratory of Bio-Inspired Materials and Interfacial Science, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.
Adv Mater. 2019 Sep;31(36):e1903029. doi: 10.1002/adma.201903029. Epub 2019 Jul 24.
Biological electrogenic systems use protein-based ionic pumps to move salt ions uphill across a cell membrane to accumulate an ion concentration gradient from the equilibrium physiological environment. Toward high-performance and robust artificial electric organs, attaining an antigradient ion transport mode by fully abiotic materials remains a great challenge. Herein, a light-driven proton pump transport phenomenon through a Janus graphene oxide membrane (JGOM) is reported. The JGOM is fabricated by sequential deposition of graphene oxide (GO) nanosheets modified with photobase (BOH) and photoacid (HA) molecules. Upon ultraviolet light illumination, the generation of a net protonic photocurrent through the JGOM, from the HA-GO to the BOH-GO side, is observed. The directional proton flow can thus establish a transmembrane proton concentration gradient of up to 0.8 pH units mm membrane area at a proton transport rate of 3.0 mol h m . Against a concentration gradient, antigradient proton transport can be achieved. The working principle is explained in terms of asymmetric surface charge polarization on HA-GO and BOH-GO multilayers triggered by photoisomerization reactions, and the consequent intramembrane proton concentration gradient. The implementation of membrane-scale light-harvesting 2D nanofluidic system that mimics the charge process of the bioelectric organs makes a straightforward step toward artificial electrogenic and photosynthetic applications.
生物电致系统利用基于蛋白质的离子泵将盐离子逆着浓度梯度跨细胞膜运输,从而在平衡的生理环境中积累离子浓度梯度。对于高性能且稳健的人造电器官而言,利用完全非生物材料实现逆梯度离子传输模式仍然是一项巨大的挑战。在此,我们报道了一种通过氧化石墨烯双面膜(JGOM)实现的光驱动质子泵运输现象。JGOM是通过依次沉积用光碱(BOH)和光酸(HA)分子修饰的氧化石墨烯(GO)纳米片制成的。在紫外光照射下,可以观察到通过JGOM产生了从HA-GO侧向BOH-GO侧的净质子光电流。因此,定向质子流能够以3.0 mol h m的质子传输速率建立高达0.8 pH单位/毫米膜面积的跨膜质子浓度梯度。克服浓度梯度,可以实现逆梯度质子运输。其工作原理可以从光异构化反应引发的HA-GO和BOH-GO多层膜上的不对称表面电荷极化以及随之产生的膜内质子浓度梯度的角度来解释。这种模拟生物电器官电荷过程的膜尺度光捕获二维纳米流体系统的实现,为人造电致和光合应用迈出了直接的一步。