Evolution of Order During Vacuum-Assisted Self-Assembly of Graphene Oxide Paper and Associated Polymer Nanocomposites

Three mechanisms are proposed for the assembly of ordered layered structures of graphene oxide, formed via the vacuum-assisted self-assembly of a dispersion of the two-dimensional nanosheets. These possible mechanisms for odering at the filter-solution interface range from regular brick-and-mortar-like growth to complete: disordered aggregation and compression. Through a series of experiments (thermal gravimetric analysis, UV-vis spectroscopy, and X-ray diffraction) a semi-ordered accumulation mechanism is identified as being dominant during paper fabrication. Additionally, a higher length-scale ordered structure (lamellae) is identified through the examination of water-swelled samples, indicating that further refinements are required to capture the complete formation mechanism. Identification of this mechanism and the resulting higher-order structure It produces provide insight Into possibilities for creation of ordered graphene. oxide-polymer nanocomposites, as well as the postfabrication madification. of single-component. graphene oxide papers.