Synthesis and investigation of acrylamide and 2-acrylamido-2-methylpropanesulfonic acid copolymer-modified graphene oxide nanomaterials with intensive viscosification capacity: An experimental and molecular dynamics study

Abstract

The polymer-modified nanomaterials with spontaneously generated cross-linked network greatly improve the dispersion viscosity, which is crucial for extending the sweep range and enhancing oil recovery. Recently, graphene oxide (GO) nanosheets have attracted extensive attention due to their high chemical reactivity and specific surface. In this paper, the AA molecule, synthesized by acrylamide (AM) and 2-acrylamido-2-methypropanesulfonic acid (AMPS) copolymerization, modified GO nanosheets (GAA) material is firstly synthesized and characterized. With the same content of AMPS segments, GAAn systems consistently exhibit better dispersion stability than AAn systems, along with higher absolute zeta potential values. The comprehensive investigation on the rheological property of GAA system reveals that GAA15 with the highest AMPS content exhibits the largest zero-shear viscosity (409.27 mPa·s) and the longest relaxation time. Based on the molecular dynamic simulation approaches, the aggregation morphology and stability of AA and GAA molecules are evaluated via the configuration analysis and the statistics of hydrogen bond numbers. The abundant binding sites from GO segments of GAA promote additional hydrogen bonds between GAA molecules and water, resulting in a more stable configuration. Molecular surface potential analysis and the independent gradient model based on Hirshfeld partition (IGMH) methods are further used to visualize the non-bonded interaction existed in cross-linked networks, which also predict and validate non-bonding interaction sites among molecular segments. The simulation results indicate higher viscosity in the GAA system should be ascribed to the formation of dispersion-strengthened cross-linked structures (AM-GO plane and GO-GO stacking segments). In summary, the microscopic viscosity-increasing mechanism of novel GAA system is proposed from the perspective of intermolecular interactions, which lays a preliminary theoretical foundation for the application of GAA material in the oil industry.