Modeling the THF clathrate hydrate dynamics by combining molecular dynamics and quasi-elastic neutron scattering

Pefoute, Eric; Martin-Gondre, L.; Ollivier, Jacques; Soetens, Jean-Christophe; Russina, Margarita; Desmedt, Arnaud

doi:10.1016/j.chemphys.2017.09.006

Cited by 6 publications

(4 citation statements)

References 67 publications

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“…Figure c shows spherically distributed THP molecules with a full quasispherical symmetry. The distribution of THF and THP molecules obtained in this study are consistent with the crystal structure model obtained by the single-crystal X-ray structure analysis , and dynamics data of THF hydrate by quasielastic neutron scattering …”

Section: Resultssupporting

confidence: 88%

“…The distribution of THF and THP molecules obtained in this study are consistent with the crystal structure model obtained by the single-crystal X-ray structure analysis 44,67 and dynamics data of THF hydrate by quasielastic neutron scattering. 68 It is also known that the smaller C 3 H 8 and iso-C 4 H 10 molecules have a spherical distribution in the 5 12 6 4 cages of the sII hydrate, 33,50,51 whereas CO 2 and C 2 H 6 in 5 12 6 2 cages of sI hydrate are distributed near the equatorial plane of the cage, with the long axis of these guests lying in the plane. 33,44,69 The distributions of guest molecules are influenced by the shape of host water cages.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

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Distortion of the Large Cages Encapsulating Cyclic Molecules and Empty Small Cages of Structure II Clathrate Hydrates

et al. 2018

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Understandings of structure-based properties of porous materials, such as gas storage and gas separation performance, are important. Here, the crystal structures of the canonical structure II (sII) clathrate hydrates encapsulating cyclic molecules (tetrahydrofuran, cyclopentane, furan, and tetrahydropyran) are studied. To understand the effect of guest molecules on the host water framework, we performed powder X-ray diffraction measurements where the hydrate structures and guest distribution within 5 12 6 4 cages were obtained by the direct-space technique followed by the Rietveld refinement. It was shown that the sizes of the 5 12 and 5 12 6 4 cages of sII hydrates expand, as its unit-cell size is enlarged by the guest. In this process, it is revealed that the shape of 5 12 6 4 cages with larger guest molecules became more spherical and volume ratio of empty small 5 12 cages in the unit cell decreases. Our findings from crystallographic point of view may give insights into better understanding of the thermodynamic stability and higher gas storage capacity of binary clathrate hydrates.

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Section: Resultssupporting

confidence: 88%

Section: ■ Experimental Sectionmentioning

confidence: 99%

Distortion of the Large Cages Encapsulating Cyclic Molecules and Empty Small Cages of Structure II Clathrate Hydrates

et al. 2018

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“…The comparison of experimental and simulated scattering data is relatively common for both X-ray and neutron scattering. Typically, a model is proposed and the comparison is made between experiment and simulation without iterative refinement of the model, for example with X-ray (Wall et al, 2014;Skinner et al, 2013;Polak et al, 2014;Megyes et al, 2004;Hura et al, 2003;Hayes et al, 2011;Ferru et al, 2014;Eggert et al, 2002;Dhungana et al, 2016;Dambournet et al, 2011;Chupas et al, 2011;Buitrago et al, 2015;Bouazizi et al, 2006) and neutron (Zeidler et al, 2014;Petridis et al, 2011;Peterson et al, 2013;Peralta et al, 2008;Pefoute et al, 2017;McNutt, Wang et al, 2014;McNutt, McDonnell et al, 2017;Le et al, 2014;Hess et al, 2009;Gutié rrez & Johansson, 2002;Furuya et al, 1994;Du & Corrales, 2007;Drewitt et al, 2011;Bañ uelos et al, 2014) scattering. In fewer cases, some element of refinement of the structural parameters is included through an iterative refinement of the model, for example with X-ray (Jalilehvand et al, 2001;Daisenberger et al, 2011) and neutron (Lynch et al, 2017;Kučerka et al, 2012;Du et al, 2009) scattering.…”

Section: Introductionmentioning

confidence: 99%

Evaluation of nano- and mesoscale structural features in composite materials through hierarchical decomposition of the radial distribution function

et al. 2018

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Composite materials possessing both crystalline and amorphous domains, when subjected to X‐ray and neutron scattering, generate diffraction patterns that are often difficult to interpret. One approach is to perform atomistic simulations of a proposed structure, from which the analogous diffraction pattern can be obtained for validation. The structure can be iteratively refined until simulation and experiment agree. The practical drawback to this approach is the significant computational resources required for the simulations. In this work, an alternative approach based on a hierarchical decomposition of the radial distribution function is used to generate a physics‐based model allowing rapid interpretation of scattering data. In order to demonstrate the breadth of this approach, it is applied to a series of carbon composites. The model is compared with atomistic simulation results in order to demonstrate that the contributions of the crystalline and amorphous domains, as well as their interfaces, are correctly captured. Because the model is more efficient, additional structural refinement is performed to increase the agreement of the simulation result with the experimental data. The model achieves a reduction in computational effort of six orders of magnitude relative to simulation. The model can be generally extended to other composite materials.

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“…In this regard, researchers have focused on the kinetics and thermodynamic properties that promote hydrate formation. In order to reduce the phase equilibrium pressure of CO 2 hydrate, tetrahydrofuran (THF) is commonly used as a thermodynamic promoter of CO 2 hydrate. , THF could decline the phase equilibrium condition of (CO 2 + THF) mixed hydrates and the induction time of hydrate formation . Lee et al studied the effect of THF on hydrate formation in a CO 2 + H 2 mixture.…”

Section: Introductionmentioning

confidence: 99%

Rapid Growth of the CO₂ Hydrate Induced by Mixing Trace Tetrafluoroethane

Song,

Zhang,

et al. 2023

ACS Omega

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Rapid formation of the CO 2 hydrate can be significantly induced by the gaseous thermodynamic promoter 1,1,1,2-tetrafluoroethane(R134a) due to the mild phase equilibrium conditions, although the formation mechanism and dynamic behavior are not clear. Therefore, a visual experimental system was developed to study the effects of different concentrations of R134a on the induction time, gas consumption, and growth morphology of the CO 2 hydrate. At the same time, the combined effects under stirring and sodium dodecyl sulfate (SDS) systems were also studied. In addition, visualization and experimental model diagrams were combined to explain the fast formation mechanism of the R134a/CO 2 hydrate. The results show that the CO 2 hydrate average conversion rate was increased by more than 63% with the addition of mixed trace R134a(7%). A special phenomenon is found that two temperature peaks appear on the hydrate formation temperature curve, corresponding to two different stages of hydrate formation when stirring or SDS is added to the mixed gas reaction system. Furthermore, the gas consumption in stirring and SDS systems increases by 9 and 44%, respectively. Finally, it is also found that the R134a/CO 2 mixed hydrate formed under the action of SDS has a "capillary" mechanism, which provides a gas− liquid phase exchange channel and a large number of nucleation sites for CO 2 hydrate, thus promoting the formation of CO 2 hydrate. This paper provides a novel, simple, and efficient method for CO 2 hydrate gas storage technology.

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Modeling the THF clathrate hydrate dynamics by combining molecular dynamics and quasi-elastic neutron scattering

Abstract: International audienc

Cited by 6 publications

References 67 publications

Distortion of the Large Cages Encapsulating Cyclic Molecules and Empty Small Cages of Structure II Clathrate Hydrates

Distortion of the Large Cages Encapsulating Cyclic Molecules and Empty Small Cages of Structure II Clathrate Hydrates

Evaluation of nano- and mesoscale structural features in composite materials through hierarchical decomposition of the radial distribution function

Rapid Growth of the CO₂ Hydrate Induced by Mixing Trace Tetrafluoroethane

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Modeling the THF clathrate hydrate dynamics by combining molecular dynamics and quasi-elastic neutron scattering

Abstract: International audienc

Cited by 6 publications

References 67 publications

Distortion of the Large Cages Encapsulating Cyclic Molecules and Empty Small Cages of Structure II Clathrate Hydrates

Distortion of the Large Cages Encapsulating Cyclic Molecules and Empty Small Cages of Structure II Clathrate Hydrates

Evaluation of nano- and mesoscale structural features in composite materials through hierarchical decomposition of the radial distribution function

Rapid Growth of the CO2 Hydrate Induced by Mixing Trace Tetrafluoroethane

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Rapid Growth of the CO₂ Hydrate Induced by Mixing Trace Tetrafluoroethane