CO2-leakage-driven diffusiophoresis causes spontaneous accumulation of charged materials in channel flow

We identify a phenomenon where the onset of channel flow creates an unexpected, charge-dependent accumulation of colloidal particles, which occurs in a common-flow configuration with gas-permeable walls, but in the absence of any installed source of gas. An aqueous suspension of either positively charged (amine-modified polystyrene; a-PS) or negatively charged (polystyrene; PS) particles that flowed into a polydimethylsiloxane (PDMS) channel created charge-dependent accumulation 2 to 4 min after the onset of flow. We unravel the phenomenon with systematic experiments under various conditions and model calculations considering permeability of the channel walls and CO2-driven diffusiophoresis. We demonstrate that such spontaneous transport of particles is driven by the gas leakage through permeable walls, which is induced by the pressure difference between the channel and the ambient. Since the liquid pressure is higher, an outward flux of gas forms in the flow. We also observe the phenomenon in a bacterial suspension of Vibrio cholerae, where the fluorescent protein (mKO; monomeric Kusabira Orange) and bacterial cells show charge-dependent separation in a channel flow. Such experimental observations show that diffusiophoresis of charged particles in an aqueous suspension can be achieved by having gas leakage through permeable walls, without any preimposed ion-concentration gradient in the liquid phase. Our findings will help resolve unexpected challenges and biases in on-chip experiments involving particles and gas-permeable walls and help understand similar configurations that naturally exist in physiological systems, such as pulmonary capillaries. We also demonstrate potential applications, such as concentrating and collecting proteins below the isoelectric point.