Graphitization of amorphous carbons: A comparative study of interatomic potentials

Tomás, Carla de; Suarez-Martinez, Irène; Marks, Nigel A.

doi:10.1016/j.carbon.2016.08.024

Cited by 212 publications

(202 citation statements)

References 76 publications

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“…This study examined the carbon hybridization, ring formation, and pore size distribution as a function of density and quench rate, and demonstrated the potential that ReaxFF could be effective in generating model CDCs; however, the study was not explicitly focused on the formation of experimentally relevant CDCs. EDIP, which has been shown to exhibit similar behavior to ReaxFF at low density [67], has been used to generate CDCs via removal of metal atoms from a carbide lattice and subsequent annealing at the target density, showing close agreement with experimental pore size distributions.…”

Section: Introductionmentioning

confidence: 68%

“…Carbon-based materials, and CDCs in particular, present a unique challenge for these forcefields because of their nanoscale heterogeneity. Individual forcefields can sufficiently describe specific structural moeities, such as short-range graphitization at low density [67], but are often not sufficient to capture the full range of non-ideal features observed in CDCs [68].…”

Section: Introductionmentioning

confidence: 99%

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

Thompson

Dyatkin

Wang

et al. 2017

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Abstract:We report a novel atomistic model of carbide-derived carbons (CDCs), which are nanoporous carbons with high specific surface areas, synthesis-dependent degrees of graphitization, and well-ordered, tunable porosities. These properties make CDCs viable substrates in several energy-relevant applications, such as gas storage media, electrochemical capacitors, and catalytic supports. These materials are heterogenous, non-ideal structures and include several important parameters that govern their performance. Therefore, a realistic model of the CDC structure is needed in order to study these systems and their nanoscale and macroscale properties with molecular simulation. We report the use of the ReaxFF reactive force field in a quenched molecular dynamics routine to generate atomistic CDC models. The pair distribution function, pore size distribution, and adsorptive properties of this model are reported and corroborated with experimental data. Simulations demonstrate that compressing the system after quenching changes the pore size distribution to better match the experimental target. Ring size distributions of this model demonstrate the prevalence of non-hexagonal carbon rings in CDCs. These effects may contrast the properties of CDCs against those of activated carbons with similar pore size distributions and explain higher energy densities of CDC-based supercapacitors.

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Section: Introductionmentioning

confidence: 68%

Section: Introductionmentioning

confidence: 99%

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

Thompson

Dyatkin

Wang

et al. 2017

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“…8 These fast potentials make large-scale moleculardynamics (MD) simulations possible, and have been applied to engineering problems such as fracture 17 or friction and wear of ta-C coatings;…”

Section: -6mentioning

confidence: 99%

“…89 its choice depends on the computational method, 8 and a suitable annealing temperature must therefore be found by trial and error.…”

mentioning

confidence: 99%

Machine learning based interatomic potential for amorphous carbon

2017

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We introduce a Gaussian approximation potential (GAP) for atomistic simulations of liquid and amorphous elemental carbon. Based on a machine-learning representation of the density-functional theory (DFT) potential-energy surface, such interatomic potentials enable materials simulations with close-to DFT accuracy but at much lower computational cost. We first determine the maximum accuracy that any finite-range potential can achieve in carbon structures; then, using a novel hierarchical set of two-, three-, and many-body structural descriptors, we construct a GAP model that can indeed reach the target accuracy. The potential yields accurate energetic and structural properties over a wide range of densities; it also correctly captures the structure of the liquid phases, at variance with state-of-the-art empirical potentials. Exemplary applications of the GAP model to surfaces of "diamond-like" tetrahedral amorphous carbon (ta-C) are presented, including an estimate of the amorphous material's surface energy, and simulations of high-temperature surface reconstructions ("graphitization"). The new interatomic potential appears to be promising for realistic and accurate simulations of nanoscale amorphous carbon structures.

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“…Our simulations use the Environment Dependent Interatomic Potential (EDIP) [41] for carbon. EDIP has been successful in MD simulations of graphitization processes [42,43,44,45,46] and in HRMC and MC models of nanoporous carbon. [36,30,47,31] To bridge the gap between the experimental and simulation timescale we develop an Arrhenius framework which allows correlation between the experimental and simulation temperatures.…”

Section: Introductionmentioning

confidence: 99%

Structural prediction of graphitization and porosity in carbide-derived carbons

Tomás

Suarez-Martinez

Vallejos-Burgos

et al. 2017

Carbon

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Carbide-derived carbons (CDCs) are nanoporous carbons with a tunable pore size, making them desirable for their adsorption properties. Despite their applicability, reliable structural models are difficult to construct due to the interplay between strong short-range order and long-range disorder. Here, a mimetic methodology is developed to generate atomistic models of CDCs using Molecular Dynamics and the Environment Dependent Interaction Potential. This approach reproduces the main characteristics of experimentally-prepared CDCs, including microstructure, porosity at the nanometre scale, and graphitization with increasing temperature. An Arrhenius-based approach is used to bridge the timescale gap between Molecular Dynamics and experiment and build a connection between the simulation and synthesis temperatures. The method is robust, easy to implement, and enables a fast exploration of the adsorption properties of CDCs.

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Graphitization of amorphous carbons: A comparative study of interatomic potentials

Cited by 212 publications

References 76 publications

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

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

Machine learning based interatomic potential for amorphous carbon

Structural prediction of graphitization and porosity in carbide-derived carbons

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