Improving the liquid phase exfoliation efficiency of graphene based on the enhanced intermolecular and interfacial interactions

The liquid phase exfoliation (LPE) technique presents significant advantages and potential for the large-scale production of high-quality graphene nanosheets (GNs) with minimal defects. Nevertheless, the Hansen solubility parameters and surface tension matched principle were limited the range of suitable solvents for LPE process. As a result, commonly employed solvents such as N-methyl-2-pyrrolidone (NMP) and N, N-Dimethylformamide (DMF) exhibit low viscosity, leading to a low transmission efficiency of shear force from solvent to graphite, resulting in inadequate shear force and low exfoliation efficiency. In this work, to break through limitations of existing solvent systems, we investigate the influence of solvent viscosity on the LPE efficiency in various pyrrolidone solvents, which share similar structures with NMP but have longer molecular chains and higher viscosity. When compared to the NMP system, the concentration of GNs in the N-octyl-2-pyrrolidone (NOP) suspension system exhibits a significant increase of approximately 70 %, which primarily attributed to the higher intermolecular and interfacial interactions in NOP suspension. More interestingly, the interactions could be further intensified by reducing the operating temperature in the NOP suspension system, which leading to an about 150 % improvement in LPE efficiency when compared to the NMP system at standard temperature. Given the remarkable conductivity of GNs, the prepared Cellulose nanofibers/graphene nanosheets (CNF/GNs) composite film exhibits lightweight and efficient electromagnetic shielding performance of 2.4 x 10(4) dB cm(2) g(-1).This work is expected to establish a universal and efficient pathway for the economical and high-yield production of GNs, elucidating the microscopic mechanism by which molecular conformation at the solid-liquid interface influences the transfer of shear forces from solvent to graphite, thereby promoting the development of widespread applications of GNs ang other two-dimensional (2D) nanomaterials.