Molecular Modeling of Microporous Structures of Carbide-Derived Carbon-Based Supercapacitors

Abstract

Microporous carbide-derived carbons are an important structural class for various technological applications. We present two possible strategies based on molecular dynamics simulations for modeling microporous amorphous carbon. In addition, we have investigated the influence of the precursor structure and simulation parameters on the porosity of the final model structure. We observed a minor influence of the precursor structure on the porosity and found that the structural properties such as pore size and hybridization in the modeled carbon structures agree well with experimental findings. Moreover, CO 2 adsorption isotherms have been simulated using Monte Carlo simulations for comparsion with experimental data. In this context, we have also considered partially oxidized carbon structures for which an increased uptake of CO 2 was observed.

Towards an atomistic understanding of disordered carbon electrode materials

“…2b ), which agrees well with EELS experiments: in so-called carbide-derived carbons (CDCs), obtained by etching titanium out of a TiC matrix, the sp 2 content is mostly >90% and increases with synthesis temperature. 7 , 16 , 29 We compare a calculated PDF to representative experiments and find that it reproduces all general features ( Fig. 2c ); see also the ESI.…”

First-principles study of alkali-metal intercalation in disordered carbon anode materials

“…Amorphous carbon 24 and silicon anodes 25 have been looked at with model DFT computations. Larger model system sizes are principally accessible to empirically fitted force fields, [26][27][28][29][30] and indeed ReaxFF type force fields have been described for Li-C phases 31 and Na intercalation; 32 however, these methods are necessarily limited by the fixed functional form of the interatomic potential, and they allow no insight into the electronic structure.…”

An Atomistic Carbide-Derived Carbon Model Generated Using ReaxFF-Based Quenched Molecular Dynamics

“…Previous QMD results have used force fields such as the Adaptive Intermolecular Reactive Empirical Bond Order (AIREBO) [61], the Environment-Dependent Interatomic Potential (EDIP) [62], the Reactive Summation State (RSS) [53], and the Tersoff potential [63] to generate nanoporous carbon structures for use in molecular simulation. While many impactful studies [49,52,54,55,[64][65][66] have been done with these forcefields, the generated structures have often failed to accurately reproduce experimental pore size distributions and always depend, at least in part, on the accuracy of the force field itself. Carbon-based materials, and CDCs in particular, present a unique challenge for these forcefields because of their nanoscale heterogeneity.…”