Abstract
Graphene oxide (GO) oligo-layered laminates were self-assembled on porous ceramic substrates via their simple dip-coating into aqueous GO dispersions. To augment the stability of the developed composite GO/ceramic membranes and control the morphology and stacking quality of the formed laminate, short-((3-glycidoxypropyl)trimethoxy silane-GLYMO, (3-aminopropyl)triethoxy silane-APTES), and long-chain (polydopamine-PDA) molecules were involved and examined as interfacial linkers. A comparative study was performed regarding the linker's capacity to enhance the interfacial adhesion between the ceramic surface and the GO deposit and affect the orientation and assemblage characteristics of the adjacent GO nanosheets that composed the formed oligo-layered laminates. Subsequently, by post-filtrating a GO/H2O suspension through the oligo-layered laminate membranes, the respective multi-layered ones have been developed, whereas ethylenediamine (EDA) was used in the suspension as an efficient molecular linker that strongly bonds and interlocks the GO nanosheets. The definition of the best linker and approach was conducted on macroporous α-alumina disks, due to the use of inexpensive raw materials and the ability to fabricate them in the lab with high reproducibility. To validate the concept at a larger scale, while investigating the effect of the porous substrate as regards its micrometer-scale roughness and surface chemistry, specific chemical modifications that yielded membranes with the best gas permeability/selectivity performance were replicated on a commercial single-channel monolith with a ZrO2 microfiltration layer. XRD, Raman, ATR, FESEM, and XPS analyses were conducted to study the structural, physicochemical, surface, and morphological properties of the GO/ceramic composite membranes, whereas permeance results of several gases at various temperatures and trans-membrane pressures were interpreted to shed light on the pore structural features. Concerning the short-chain linkers, the obtained results ascertain that GLYMO causes denser and more uniform assembly of GO nanosheets within the oligo-layered laminate. PDA had the same beneficial effect, as it is a macromolecule. Overall, this study shows that the development of gas-separating membranes, by just dipping the linker-modified substrate into the GO suspension, is not straightforward. The application of post-filtration contributed significantly to this target and the quality of the superficially deposited, thick GO laminate depended on this of the chemically attached oligo-layered one.