Interplay between membrane imperfections and external concentration polarization

Abstract

Reverse osmosis membranes provide a highly effective and efficient barrier against various kinds of pollutants. Their reliability depends on the integrity of the active layer: in case the active layer is damaged and contains imperfections, unfiltered feed solution can contaminate the permeate. Various types of integrity monitoring techniques have been developed to verify membrane performance, of which the rejection of fluorescent dyes is a well-established technique. Fluorescent dyes are however relatively small solutes for which the membranes can display non-zero diffusive permeability, such that not all dye passage can be attributed to membrane imperfections. Additionally, fluorescent dyes are subject to external concentration polarization (ECP) during filtration, causing a flux-dependent enrichment at the membrane surface, further complicating the analysis of dye rejection data. This study presents a model to discern between membrane permeability, enrichment by ECP and passage through imperfections. The consequences of imperfections on solute passage are explored, showing that imperfections only contribute significantly to the passage of solutes with a low membrane permeability. This leads to underestimates of the external mass transfer coefficient, with the error being increasingly large with decreasing membrane permeability coefficient, relative to the case of an imperfection-free membrane. This error is then related to the proportionality of the Sherwood number, used to calculate external mass transfer coefficients, with solute diffusivity, allowing the quantification of the contribution of imperfections to water flux. The model was experimentally verified using Pyranine rejection in two membrane types, both operated in a lab-scale flat sheet crossflow test system, finding proof of imperfections in one membrane type.