pH-Dependent Zeta Potential Induces Diffusiophoretic Focusing in an Acid-Base Reaction

Abstract

Diffusiophoresis of charged particles in the presence of electrolytes has been extensively studied in the literature. However, in these setups, particles typically move in a single direction, either up or down the electrolyte gradient. Here, we theoretically investigate the conditions under which a particle can reverse its diffusiophoretic direction within the same setup, leading to the formation of a focusing band under steady-state concentration gradients. Using multi-ion diffusiophoresis calculations, we simulate particle transport in an acid-based reaction system where salt is added alongside the acid. For a range of salt concentrations, particles focus within the channel. Our analysis reveals that a pH-dependent zeta potential is necessary for this focusing to occur, and determines where the particles focus, i.e., on or off the acid-base reaction front. We report qualitative agreement with prior experimental observations and derive analytical conditions governing particle focusing, highlighting the delicate balance between concentration gradients and zeta potential variations. The work elucidates the crucial physics of pH-dependent zeta potential and opens new avenues for exploring diffusiophoresis in acid-base systems, with implications for microfluidic design and biophysical transport processes.