Computational Microscopy of PEDOT:PSS/Cellulose Composite Paper

Abstract

Organic composite cellulose/conducting polymer materials have recently demonstrated their potential for energy storage applications. Here, we report a computational morphological study of CNF-PEDOT paper, which is composed of cellulose nanofibers (CNFs), and conducting polymer poly­(3,4-ethylenedioxythiophene) blended with poly­(styrenesulfonate) (PEDOT:PSS). With use of coarse-grained MARTINI molecular dynamics simulations, we study the aggregation of PEDOT:PSS on the cellulose surface, exploring different initial conditions for the self-assembly. The orientation of PEDOT chains with respect to the cellulose surface was studied, and the diffraction patterns were simulated. Finally, available experimental data were discussed and compared with calculated morphological models.

A novel supra coarse-grained model for cellulose

“…In the current section, we present ''water'' evaporation simulations prepared with our sCG model. Since in our approach we use an implicit solvent MD simulation, the solvent evaporation can not be done in the usual way as in the explicit solvent MD, where solvent molecules are removed individually (Mehandzhiyski and Zozoulenko 2019). For our simulations the system was prepared by randomly placing 200 CNC with length 100 nm in a simulation box with the periodic boundary condition with a side of 300 nm, shown in Fig.…”

“…Cellulose has been the subject of many molecular simulation studies. Some of these studies focus only at the surface phenomena and modifications of CNC, (Chen et al 2017;Zhou et al 2015;Bergenstråhle et al 2008;Paajanen et al 2016;Chundawat et al 2011) while many others simulate whole CNC, both at atomistic (Chen et al 2017;Zhou et al 2015;Bergenstråhle et al 2008;Paajanen et al 2016;Chundawat et al 2011;Matthews et al 2006;Conley et al 2016;Oehme et al 2015;Djahedi et al 2015;Paajanen et al 2019;Ciesielski et al 2019) and coarsegrained representations (López et al 2009;Wohlert and Berglund 2011;López et al 2015;Mehandzhiyski and Zozoulenko 2019;Glass et al 2012;Fan and Maranas 2015;Markutsya et al 2013;Shishehbor et al 2018;Shishehbor and Zavattieri 2019;Ramezani and Golchinfar 2019;Srinivas et al 2011;Poma et al 2015Poma et al , 2016Poma et al , 2017. All-atom molecular dynamics (AA-MD) studies are able to simulate the crystal structure of cellulose in a perfect agreement with the experimental crystal structure of different cellulose allomorphs and provide a detailed atomistic picture for the structure and dynamics of CNC (Chundawat et al 2011).…”

“…Several CG models for CNC have been developed through the years. They have different degree of mapping (grouping the atoms from the atomistic model in one interaction bead) varying from 4 heavy atoms mapped into one CG bead, in the case of the most popular CG force field, MARTINI, (López et al 2009;Wohlert and Berglund 2011;López et al 2015;Mehandzhiyski and Zozoulenko 2019) to 1 or even 2 glucose units represented by 1 CG bead (Glass et al 2012;Fan and Maranas 2015;Markutsya et al 2013;Shishehbor et al 2018; Shishehbor and Zavattieri 2019; Ramezani and Golchinfar 2019). These approaches help to decrease the computational cost of the simulations and enable one to explore much larger systems, but sacrifices the fine atomistic details presented in the AA models.…”

Ambient‐Dried, 3D‐Printable and Electrically Conducting Cellulose Nanofiber Aerogels by Inclusion of Functional Polymers

“…PEDOT and CNFs have been combined to prepare a variety of organic electronic devices; an exemplary work of this was published by Malti et al in which the PEDOT‐CNF composite displayed unprecedented high conductivity of both ions and electrons . Recent studies also show that PEDOT can self‐assemble into interconnected, highly‐conducting structures along CNFs …”

“…[53,54] Recent studies also show that PEDOT can self-assemble into interconnected, highly-conducting structures along CNFs. [55,56] This study presents a novel and environment friendly method to prepare wet-stable organic aerogels. Gels of carboxymethylated CNFs and alginate were prepared at different ionic strengths and with countercations of different valencies.…”