Influences of carboxyl functionalization of intercalators on exfoliation of graphite oxide: a molecular dynamics simulation

Choi, Hoi Kil; Oh, Yuna; Jung, Ha Yoon; Hong, Hyunkee; Ku, Bon‐Cheol; You, Nam‐Ho; Kim, Young‐Kwan; Shin, Eui Sup; Yu, Jaesang

doi:10.1039/c8cp05436c

Cited by 16 publications

(8 citation statements)

References 38 publications

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“…This yielded an interlayer spacing for G and GO equal to 0.36 and 0.59 nm, respectively. This interlayer distance for G is in good agreement with previously reported values, 87 while that for GO is in agreement with previously reported values from MD simulations 88 and experiments. 21 The AA G and GO systems consisted of 10 layers each having 836 and 1544 atoms, spanning a basal plane with dimensions of 4.6 × 4.7 nm 2 and 4.8 × 4.7 nm 2 , respectively.…”

Section: Simulation Methodssupporting

confidence: 93%

Molecular Dynamics Simulation of the n-Octacosane–Water Mixture Confined in Graphene Mesopores: Comparison of Atomistic and Coarse-Grained Calculations and the Effect of Catalyst Nanoparticle

et al. 2021

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Fischer−Tropsch synthesis (FTS) is used extensively in the gas-to-liquids (GTL) process to produce clean, highquality low emission transportation fuels from synthesis gas. In order to gain a better understanding of the phase behavior of the produced wax−water mixtures at reaction conditions by accounting for confinement effects of either hydrophilic or hydrophobic characteristics and catalyst nanoparticles (NPs), one needs to closely examine the validity of incorporating coarse grained approaches in the context of FTS. The present study focuses on simulating by means of atomistic (AA) and coarse-grained (CG) molecular dynamics (MD; CGMD) simulations the n-octacosane (n-C 28 )−water mixture inside graphene (G) and graphene oxide (GO) mesopores under low-temperature FTS conditions (473.15 K) with the inclusion of a Co NP. Graphene derivatives were selected as they are emerging catalyst support materials in the FTS reaction and allow for direct comparisons between the AA and CG methodologies. We also evaluated the presence of long-chain alcohols such as dodecan-1-ol at 7 wt % on the n-C 28 −H 2 O mixture phase behavior. The AA simulations involved the use of the united atom TraPPE (TraPPE-UA) force field for n-C 28 and the alcohols and the TIP4P/2005 force field for water, while the MARTINI force field was used for the CG description. With regard to the mixtures inside the G pore, both AA and CG simulation methods capture the phase separation of the mixture, with water molecules occupying the center of the pore and n-C 28 forming layers at the pore walls; inside GO, both methodologies show that water separates near the surface and the model wax lies at the pore center. Both AA and CG simulations accurately capture the n-C 28 and H 2 O diffusivity as a function of the distance from the G and GO pore centers, respectively, being lower closer to the pore surface. Dodecan-1-ol is mostly located at the n-C 28 −H 2 O interface showing a higher preference toward the wax as a consequence of increased van der Waals intermolecular interactions, slightly reducing the mobility of water. The agreement between AA and CG MD simulations paved the way for novel CGMD simulations with DFT-derived parameters for Co, to study the n-C 28 −H 2 O behavior in its presence. Our results show that the Co NP does not affect phase separation of the n-C 28 −H 2 O mixture inside the pores; however, water at such high concentrations covers the Co NP surface extensively. Given the experimental difficulties in exploring the relevant mechanisms at this scale, our results showcase that CGMD using the MARTINI force field can be employed to study FTS-related processes at this level and are expected to open new pathways in the investigation of confined mixtures relevant to the FTS reaction in the presence of supported catalyst NPs.

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Section: Simulation Methodssupporting

confidence: 93%

Molecular Dynamics Simulation of the n-Octacosane–Water Mixture Confined in Graphene Mesopores: Comparison of Atomistic and Coarse-Grained Calculations and the Effect of Catalyst Nanoparticle

et al. 2021

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“…There are a large number of carboxyl groups at the edge of graphene oxide, and the carboxyl group is a highly reactive group, and thus has been greatly studied for the functionalization of graphene oxide. 81,82 The carboxyl functionalization step is generally the activation of the reaction, and then the group containing an amino group and a hydroxyl group is dehydrated to form an ester or amide bond. The reagents commonly used for carboxyl activation include thionyl chloride (SOCl 2 ), 83 2-(7-aza-1H-benzotriazole-1yl)-1,1,3,3-tetramethyluronium hexauorophosphate, 84 N,Ndicyclohexylcarbodiimide (DCC), 85 and 1-ethyl-3-(3dimethylaminopropyl)-carbodiimide (EDC).…”

Section: Covalent Functionalizationmentioning

confidence: 99%

Progress in the functional modification of graphene/graphene oxide: a review

et al. 2020

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“…Carboxyl groups have already been extensively inspected in graphene materials, [135][136][137] and owing to the similar surface chemistry environment, it is possible to introduce carboxyl groups into MXene materials. [112][113][114] Similar to amino groups, carboxyl groups can be applied to a couple of chemicals via the aforementioned interaction with amino groups to form amides or esters.…”

Section: Carboxyl Group (-Cooh)mentioning

confidence: 99%

Surface engineering of MXenes for energy and environmental applications

Tong

et al. 2022

J. Mater. Chem. A

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Influences of carboxyl functionalization of intercalators on exfoliation of graphite oxide: a molecular dynamics simulation

Abstract: In this study, the influences of the carboxyl functionalization of intercalators on exfoliation of graphite oxide were analyzed using molecular dynamics (MD) simulations.

Cited by 16 publications

References 38 publications

Molecular Dynamics Simulation of the n-Octacosane–Water Mixture Confined in Graphene Mesopores: Comparison of Atomistic and Coarse-Grained Calculations and the Effect of Catalyst Nanoparticle

Molecular Dynamics Simulation of the n-Octacosane–Water Mixture Confined in Graphene Mesopores: Comparison of Atomistic and Coarse-Grained Calculations and the Effect of Catalyst Nanoparticle

Progress in the functional modification of graphene/graphene oxide: a review

Surface engineering of MXenes for energy and environmental applications

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