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We present a microfluidic method leading to accurate measurements of the mutual diffusion coefficient of a liquid binary mixture over the whole solute concentration range in a single experiment. This method fully exploits solvent pervaporation through a poly(dimethylsiloxane) (PDMS) membrane to obtain a steady concentration gradient within a microfluidic channel. Our method is applicable for solutes which cannot permeate through PDMS, and requires the activity and the density over the full concentration range as input parameters. We demonstrate the accuracy of our methodology by measuring the mutual diffusion coefficient of the water (1) + glycerol (2) mixture, from measurements of the concentration gradient using Raman confocal spectroscopy and the pervaporation‐induced flow using particle tracking velocimetry. © 2017 American Institute of Chemical Engineers  AIChE J , 63: 358–366, 2018

Steady microfluidic measurements of mutual diffusion coefficients of liquid binary mixtures