Bafna Jayesh A, Pangeni Sushil, Winterhalter Mathias, Aksoyoglu M Alphan
Department of Life Sciences and Chemistry, Jacobs University, Bremen, Germany.
Department of Life Sciences and Chemistry, Jacobs University, Bremen, Germany.
Biophys J. 2020 Jun 2;118(11):2844-2852. doi: 10.1016/j.bpj.2020.04.011. Epub 2020 Apr 19.
We report that the dynamics of antibiotic capture and transport across a voltage-biased OmpF nanopore is dominated by the electroosmotic flow rather than the electrophoretic force. By reconstituting an OmpF porin in an artificial lipid bilayer and applying an electric field across it, we are able to elucidate the permeation of molecules and their mechanism of transport. This field gives rise to an electrophoretic force acting directly on a charged substrate but also indirectly via coupling to all other mobile ions, causing an electroosmotic flow. The directionality and magnitude of this flow depends on the selectivity of the channel. Modifying the charge state of three different substrates (norfloxacin, ciprofloxacin, and enoxacin) by varying the pH between 6 and 9 while the charge and selectivity of OmpF is conserved allows us to work under conditions in which electroosmotic flow and electrophoretic forces add or oppose. This configuration allows us to identify and distinguish the contributions of the electroosmotic flow and the electrophoretic force on translocation. Statistical analysis of the resolvable dwell times reveals rich kinetic details regarding the direction and the stochastic movement of antibiotics inside the nanopore. We quantitatively describe the electroosmotic velocity component experienced by the substrates and their diffusion coefficients inside the porin with an estimate of the energy barrier experienced by the molecules caused by the interaction with the channel wall, which slows down the permeation by several orders of magnitude.
我们报告称,抗生素在电压偏置的OmpF纳米孔中的捕获和传输动力学主要由电渗流而非电泳力主导。通过在人工脂质双层中重构OmpF孔蛋白并在其上施加电场,我们能够阐明分子的渗透及其传输机制。该电场会产生直接作用于带电底物的电泳力,也会通过与所有其他移动离子的耦合间接产生电泳力,从而导致电渗流。这种流动的方向性和大小取决于通道的选择性。在保持OmpF的电荷和选择性不变的情况下,通过在6至9之间改变pH值来改变三种不同底物(诺氟沙星、环丙沙星和依诺沙星)的电荷状态,使我们能够在电渗流和电泳力相加或相抵的条件下开展工作。这种配置使我们能够识别和区分电渗流和电泳力对转运的贡献。对可分辨停留时间的统计分析揭示了纳米孔内抗生素方向和随机运动的丰富动力学细节。我们定量描述了底物所经历的电渗速度分量及其在孔蛋白内的扩散系数,并估计了分子与通道壁相互作用所经历的能垒,这使渗透速度减慢了几个数量级。