Atomistic Scale Analysis of the Carbonization Process for C/H/O/N-Based Polymers with the ReaxFF Reactive Force Field

Malgorzata Kowalik, Chowdhury Ashraf, Behzad Damirchi, Dooman Akbarian, Siavash Rajabpour, Adri C.T. Van Duin

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

During the carbonization process of raw polymer precursors, graphitic structures can evolve. The presence of these graphitic structures affects mechanical properties of the carbonized carbon fibers. To gain a better understanding of the chemistry behind the evolution of these structures, we performed atomistic-scale simulations using the ReaxFF reactive force field. Three different polymers were considered as a precursor: idealized ladder PAN (polyacrylonitrile), a proposed oxidized PAN, and poly(p-phenylene-2,6-benzobisoxazole). We determined the underlying molecular details of polymer conversion into a carbon fiber structure. Because these are C/H/O/N-based polymers, we first developed an improved force field for C/H/O/N chemistry based on the density functional theory data with a particular focus on N2 formation kinetics and its interactions with polymer-associated radicals formed during the carbonization process. Then, using this improved force field, we performed atomistic-scale simulations of the initial stage of the carbonization process for the considered polymers. On the basis of our simulation data, the molecular pathways for the formation of low-molecular-weight gas species and all-carbon ring formation were determined. We also examined the possible alignment of the developed all-carbon 6-membered ring clusters, which is crucial for the further graphitic structure evolution.

Original languageEnglish (US)
JournalJournal of Physical Chemistry B
DOIs
StatePublished - Jan 1 2019

Fingerprint

carbonization
Carbonization
field theory (physics)
Polymers
polymers
polyacrylonitrile
Polyacrylonitriles
carbon fibers
Carbon fibers
Carbon
chemistry
carbon
rings
Ladders
data simulation
low molecular weights
ladders
Density functional theory
simulation
Gases

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

Cite this

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title = "Atomistic Scale Analysis of the Carbonization Process for C/H/O/N-Based Polymers with the ReaxFF Reactive Force Field",
abstract = "During the carbonization process of raw polymer precursors, graphitic structures can evolve. The presence of these graphitic structures affects mechanical properties of the carbonized carbon fibers. To gain a better understanding of the chemistry behind the evolution of these structures, we performed atomistic-scale simulations using the ReaxFF reactive force field. Three different polymers were considered as a precursor: idealized ladder PAN (polyacrylonitrile), a proposed oxidized PAN, and poly(p-phenylene-2,6-benzobisoxazole). We determined the underlying molecular details of polymer conversion into a carbon fiber structure. Because these are C/H/O/N-based polymers, we first developed an improved force field for C/H/O/N chemistry based on the density functional theory data with a particular focus on N2 formation kinetics and its interactions with polymer-associated radicals formed during the carbonization process. Then, using this improved force field, we performed atomistic-scale simulations of the initial stage of the carbonization process for the considered polymers. On the basis of our simulation data, the molecular pathways for the formation of low-molecular-weight gas species and all-carbon ring formation were determined. We also examined the possible alignment of the developed all-carbon 6-membered ring clusters, which is crucial for the further graphitic structure evolution.",
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Atomistic Scale Analysis of the Carbonization Process for C/H/O/N-Based Polymers with the ReaxFF Reactive Force Field. / Kowalik, Malgorzata; Ashraf, Chowdhury; Damirchi, Behzad; Akbarian, Dooman; Rajabpour, Siavash; Van Duin, Adri C.T.

In: Journal of Physical Chemistry B, 01.01.2019.

Research output: Contribution to journalArticle

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AU - Kowalik, Malgorzata

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AU - Damirchi, Behzad

AU - Akbarian, Dooman

AU - Rajabpour, Siavash

AU - Van Duin, Adri C.T.

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