Templating Effect of Graphene/Graphene Oxide on the Self‐Organization of Conducting Polymers

A comprehensive study for the self-organization of conducting polymers (CPs) on graphene (Gr) and graphene oxide (GrO) surfaces is conducted through molecular dynamics (MD) simulations. Poly(3,4-ethylenedioxythiophene) (PEDOT), polythiophene (PTH), polypyrrole (PPY), and two different donor-acceptor type CPs are studied on the Gr/GrO surfaces. Self-organization of the CP chains is elucidated in different studies: self-organization of the CPs on periodic Gr/GrO surfaces at small and large scales and layer formation driven by self-organization on Gr/GrO surfaces with alternating oxygen-to-carbon atom ratios. During the adsorption of CPs, enhancement in the π-stacking of polymer chains is observed at the Gr/GrO interface, affecting further chain organizations layer by layer. Concentration and density profiles and radial distribution function (RDF) analysis of the MD simulations are used to explain self-organization of chains, quantitatively. More surface coverage and better chain packing are obtained with less oxidized GrO surfaces due to weak interfacial interaction with CPs formed via π-π stacking, van der Waals forces, and hydrophobic interactions at the interface, which may result in high chain mobility at the interface.