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Electrospray deposition (ESD) uses strong electric fields applied to solutions and dispersions exiting a capillary to produce charged monodisperse droplets driven toward grounded targets. Self‐limiting electrospray deposition (SLED) is a phenomenon in which highly directed, uniform, and even 3D coatings can be achieved by trapping charge in the deposited film, redirecting the field lines to uncoated regions of the target. However, when inorganic particles are added to SLED sprays, the buildup of charge required to repel incoming material is disrupted as particle loading increases. Due to its fibril gelling behavior, methylcellulose (MC) SLED can form nanowire morphologies. These wires, when used as a binder, can separate particles and prevent percolation. In this work, a variety of conductive and insulating particles are explored using patterned and un‐patterned substrates. This exploration allows us to maximally load particles for high‐concentration and highly controlled self‐limiting functional sprays. This is demonstrated using Ti3C2Tx MXene to functionalize an interdigitated electrode for use as a supercapacitor. 

Electrospray deposition (ESD) uses strong electric fields to produce generations of monodisperse droplets from solutions and dispersions that are driven toward grounded substrates. When soft materials are delivered, the behavior of the growing film depends on the film’s ability to dissipate charge, which is strongly tied to its mobility for dielectric materials. Accordingly, there exist three regimes of electrospray: electrowetting, charged melt, and self-limiting. In the self-limiting regime, it has been recently shown that the targeted nature of these sprays allows for corona-free 3D coating. While ESD patterning on the micron-scale has been studied for decades, most typically through the use of insulating masks, there has been no comparative study of this phenomenon across spray regimes. Here, we used test-patterns composed of gratings that range in both feature size (30–240 μm) and spacing (⅓x–9x) to compare materials across regimes. The sprayed patterns were scanned using a profilometer, and the density, average height, and specificity were extracted. From these results, it was demonstrated that material deposited in the self-limiting regime showed the highest uniformity and specificity on small features as compared to electrowetting and charged melt sprays. Self-limiting electrospray deposition is, therefore, the best suited for modification of prefabricated electrode patterns. 

Abstract Electrospray deposition (ESD) applies a high voltage to liquids flowing through narrow capillaries to produce monodisperse generations of droplets down to hundreds of nanometers in diameter, each carrying a small amount of the delivered solute. This deposition method has been combined with insulated stencil masks for fabricating micropatterns by spraying solutions containing nanoparticles, polymers, or biomaterials. To optimize the fabrication process for micro-coatings, a self-limiting electrospray deposition (SLED) method has recently been developed. Here, we combine SLED with a pre-existing patterned polymer film to study SLED’s fundamental behavior in a bilayer geometry. SLED has been observed when glassy insulating materials are sprayed onto conductive substrates, where a thickness-limited film forms as charge accumulates and repels the arrival of additional charged droplets. In this study, polystyrene (PS), Parylene C, and SU-8 thin films of varying thickness on silicon are utilized as insulated spraying substrates. Polyvinylpyrrolidone (PVP), a thermoplastic polymer is sprayed below its glass transition temperature (T g ) to investigate the SLED behavior on the pre-deposited insulating films. Furthermore, to examine the effects of in-plane confinement on the spray, a microhole array patterned onto the PS thin film by laser dewetting was sprayed with dyed PVP in the SLED mode. This was then extended to an unmasked electrode array showing that masked SLED and laser dewetting could be used to target microscale regions of conventionally-patterned electronics.