Gelation-Assisted Layer-by-Layer Deposition of High Performance Nanocomposites

Layer-by-layer (LBL) assembly produces nanocomposites with distinctively high volume fractions of nanomaterials and nanometer scale controlled uniformity. Although deposition of one nanometer scale layer at a time leads to high performance composites, this deposition mode is also associated with the slow multilayer build-up. Exponential LBL, spin coating, turbo-LBL and other methods tremendously accelerate the multilayer build-up but often yield lower, strength, toughness, conductivity, etc. Here, we introduce gelation assisted layer-by-layer (gaLBL) deposition taking advantage of a repeating cycle of hydrogel formation and subsequent polymer infiltration demonstrated using aramid nanofiber (ANF) and epoxy resin (EPX) as deposition partners. Utilization of ANF gels increases the thickness of each deposited layer from 1–10 nm to 30–300 nm while retaining fine control of thickness in each layer, high volume fraction, and uniformity. While increasing the speed of the deposition, the high density of interfaces associated with nanofiber gels helps retain high mechanical properties. The ANF/EPX multilayer composites revealed a rare combination of properties that was unavailable in traditional aramid-based and other composites, namely, high ultimate strength of 505±47 MPa, high toughness of 50.1±9.8 MJ/m3, and high transparency. Interestingly, the composite also displayed close-to-zero thermal expansion. The constellation of these materials properties is unique both for quasi-anisotropic composites and unidirectional materials with nanofiber alignment. gaLBL demonstrates the capability to resolve the fundamental challenge between high-performance and scalability. The gelation-assisted layered deposition can be extended to other functional components including nanoparticle gels.