Experimental and theoretical study of the effect of different functionalities of graphene oxide/polymer composites on selective CO(2) capture

There is a constant need for versatile technologies to reduce the continuously increasing concentration of CO(2) in the atmosphere, able to provide effective solutions under different conditions (temperature, pressure) and composition of the flue gas. In this work, a combination of graphene oxide (GO) and functionalized waterborne polymer particles was investigated, as versatile and promising candidates for CO(2) capture application, with the aim to develop an easily scalable, inexpensive, and environmentally friendly CO(2) capture technology. There are huge possibilities of different functional monomers that can be selected to functionalize the polymer particles and to provide CO(2)-philicity to the composite nanostructures. Density functional theory (DFT) was employed to gain a deeper understanding of the interactions of these complex composite materials with CO(2) and N(2) molecules, and to build a basis for efficient screening for functional monomers. Estimation of the binding energy between CO(2) and a set of GO/polymer composites, comprising copolymers of methyl methacrylate, n-butyl acrylate, and different functional monomers, shows that it depends strongly on the polymer functionalities. In some cases, there is a lack of cooperative effect of GO. It is explained by a remarkably strong GO-polymer binding, which induced less effective CO(2)-polymer interactions. When compared with experimental results, in the cases when the nanocomposite structures presented similar textural properties, the same trends for selective CO(2) capture over N(2) were attained. Besides novel functional materials for CO(2) capture and a deeper understanding of the interactions between CO(2) molecules with various materials, this study additionally demonstrates that DFT calculations can be a shorter route toward the efficient selection of the best functionalization of the composite materials for selective CO(2) capture.