Center for Nonlinear Phenomena and Complex Systems, Université Libre de Bruxelles, Code Postal 231, Campus Plaine, B-1050 Brussels, Belgium.
Chemical Physics Theory Group, Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
J Chem Phys. 2018 Apr 7;148(13):134104. doi: 10.1063/1.5020442.
The propulsion of active particles by self-diffusiophoresis is driven by asymmetric catalytic reactions on the particle surface that generate a mechanochemical coupling between the fluid velocity and the concentration fields of fuel and product in the surrounding solution. Because of thermal and molecular fluctuations in the solution, the motion of micrometric or submicrometric active particles is stochastic. Coupled Langevin equations describing the translation, rotation, and reaction of such active particles are deduced from fluctuating chemohydrodynamics and fluctuating boundary conditions at the interface between the fluid and the particle. These equations are consistent with microreversibility and the Onsager-Casimir reciprocal relations between affinities and currents and provide a thermodynamically consistent basis for the investigation of the dynamics of active particles propelled by diffusiophoretic mechanisms.
由自扩散泳驱动的活性粒子的推进是由粒子表面上的不对称催化反应驱动的,该反应在流体速度和周围溶液中燃料和产物浓度场之间产生机械化学耦合。由于溶液中的热和分子波动,微米或亚微米活性粒子的运动是随机的。从化学流体动力学和流体与粒子界面处的波动边界条件推导出描述这种活性粒子的平移、旋转和反应的耦合朗之万方程。这些方程与微观可逆性以及亲和势和电流之间的昂萨格-卡西米尔倒易关系一致,为研究由扩散泳机制推动的活性粒子的动力学提供了热力学一致的基础。