Liquid Phase Exfoliation (LPE) of graphite has been proposed as a scalable and low-cost method for graphene (G) production (A. O’Neill, U. Khan et al. Phys. Chem. C, 115, 5422–5428 (2011)). Ultrasonic mixing coupled with polymeric stabilizers effectively overcomes Van Der Walls forces between graphitic planes and isolating graphene flakes. The absence of strong oxidizing/reducing agents in the synthesis process allows the graphenic basal plane to preserve its sp2 character, with defects mainly concentrated at the flakes’ edges. In this work, we investigate the use of biocompatible solvents, ethanol (EtOH) and water, and stabilizing agents (cellulose acetate butyrate, CAB) to form stable liquid dispersions of graphene. Centrifugation of the EtOH/CAB/G mixture and removal of excess polymeric stabilizer followed the Ultrasonic Assisted Liquid Phase Exfoliation (UALPE) to obtain an optimal graphene dispersion. The resulting material is employed for the self-assembly-driven deposition of multi-layer graphene films on SiO2/Si substrates. According to the Marangoni effect principle, the low surface tension value of the graphene liquor can be exploited to induce a mass flow at the interface with a secondary high surface tension solvent (H2O). This phenomenon results in the formation of stable films of “compressed” graphene (X. Li et al., Adv. Funct. Mater., 26, 1322–1329 (2016)). Said material is deposited on the Si/SiO2 surface by a Langmuir-Shaefer/Blodgett hybrid approach with an ad hoc 3D printed sample holder. The graphene films are characterized via Raman, XPS, and SEM. Raman spectroscopy was the primary tool for the evaluation of the quality of graphene and its characteristics. The I(D)/I(G) and I(D)/I(D’) ratios confirm low-defectivity concentrated at the edges. The 2D peak shape and fit were instead used to indicate the number of graphene layers, estimated at 5-7. The same parameters were employed to analyze multi-layer graphene films, identifying the stacking of the material as electronically decoupled. The electrical properties are analyzed as a function of the coating iterations and UALPE duration to obtain conductivity data, showing the best results to be in the range of the 103 Sm.Electrochemical characterization of the deposits is evaluated by redox probing graphene in an appropriate electrolyte. A coordination complex couple like ferro/ferricyanide is used to evaluate the electrochemical performance of the graphene films as electrodes in standard cyclic voltammetry. The reversible nature of the [Fe(CN)6]3-/[Fe(CN)6]4- redox reaction allows the calculation of the Electrochemical Surface Area (ESA) by analyzing the voltammetric current1. (Y. Lei et al., J. Electroanal. Chem., 887, 115084 (2021)). The exfoliation parameters and iterations of self-assembly-driven electrode fabrication are related to the electrochemically active surface area (D. A. C. Brownson and C. E. Banks, The Handbook of Graphene Electrochemistry, p. 201, Springer London, London, (2014)). Electrochemical AFM (EC-AFM) is also utilized to assess the behavior of the carbonaceous deposits. EC-AMF in situ analysis is employed to investigate the evolution of the electrochemical phenomena on a micro/nanoscale and trace a correlation between the graphene synthesis variables and the response of the multi-layer graphene films.
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