Flow-based assembly of layer-by-layer capsules through tangential flow filtration

Layer-by-layer (LbL) assembly on nano- and microparticles is of interest for a range of applications, including catalysis, optics, sensors, and drug delivery. One current limitation is the standard use of manual, centrifugation-based (pellet/resuspension) methods to perform the layering steps, which can make scalable, highly controllable, and automatable production difficult to achieve. Here, we develop a fully flow-based technique using tangential flow filtration (TFF) for LbL assembly on particles. We demonstrate that multilayered particles and capsules with different sizes (from micrometers to submicrometers in diameter) can be assembled on different templates (e.g., silica and calcium carbonate) using several polymers (e.g., poly(allylamine hydrochloride), poly(styrenesulfonate), and poly(diallyldimethylammonium chloride)). The full system only contains fluidic components routinely used (and automated) in industry, such as pumps, tanks, valves, and tubing in addition to the TFF filter modules. Using the TFF LbL system, we also demonstrate the centrifugation-free assembly, including core dissolution, of drug-loaded capsules. The well-controlled, integrated, and automatable nature of the TFF LbL system provides scientific, engineering, and practical processing benefits, making it valuable for research environments and potentially useful for translating LbL assembled particles into diverse applications.