Probing the Hydrogen Equilibrium and Kinetics in Zeolite Iimidazolate Frameworks via Molecular Dynamics and Quasi-Elastic Neutron Scattering Experiments Научная публикация
| Журнал |
Journal of Chemical Physics
ISSN: 0021-9606 , E-ISSN: 1089-7690 |
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| Вых. Данные | Год: 2013, Том: 138, Номер: 3, Страницы: 034706 Страниц : 10 DOI: 10.1063/1.4774375 | ||||||||
| Ключевые слова | Deuterium; Diffusion; Experiments; Hydrogen; Monte Carlo methods; Neutron scattering; Phase equilibria; Quantum theory; Sorption | ||||||||
| Авторы |
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| Организации |
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Информация о финансировании (1)
| 1 | European Commission | 233502 FP7-NMP-2008-EU-India-2 AMCOS |
Реферат:
The problem of simulating processes involving equilibria and dynamics of guest sorbates within zeolitic imidazolate frameworks (ZIF) by means of molecular dynamics (MD) computer experiments is of growing importance because of the promising role of ZIFs as molecular "traps" for clean energy applications. A key issue for validating such an atomistic modeling attempt is the possibility of comparing the MD results, with real experiments being able to capture analogous space and time scales to the ones pertained to the computer experiments. In the present study, this prerequisite is fulfilled through the quasi-elastic neutron scattering technique (QENS) for measuring self-diffusivity, by elaborating the incoherent scattering signal of hydrogen nuclei. QENS and MD experiments were performed in parallel to probe the hydrogen motion, for the first time in ZIF members. The predicted and measured dynamics behaviors show considerable concentration variation of the hydrogen self-diffusion coefficient in the two topologically different ZIF pore networks of this study, the ZIF-3 and ZIF-8. Modeling options such as the flexibility of the entire matrix versus a rigid framework version, the mobility of the imidazolate ligand, and the inclusion of quantum mechanical effects in the potential functions were examined in detail for the sorption thermodynamics and kinetics of hydrogen and also of deuterium, by employing MD combined with Widom averaging towards studying phase equilibria. The latter methodology ensures a rigorous and efficient way for post-processing the dynamics trajectory, thereby avoiding stochastic moves via Monte Carlo simulation, over the large number of configurational degrees of freedom a nonrigid framework encompasses.
Библиографическая ссылка:
Pantatosaki E.
, Jobic H.
, Kolokolov D.I.
, Karmakar S.
, Biniwale R.
, Papadopoulos G.K.
Probing the Hydrogen Equilibrium and Kinetics in Zeolite Iimidazolate Frameworks via Molecular Dynamics and Quasi-Elastic Neutron Scattering Experiments
Journal of Chemical Physics. 2013. V.138. N3. P.034706. DOI: 10.1063/1.4774375 WOS Scopus РИНЦ CAPlusCA OpenAlex
Probing the Hydrogen Equilibrium and Kinetics in Zeolite Iimidazolate Frameworks via Molecular Dynamics and Quasi-Elastic Neutron Scattering Experiments
Journal of Chemical Physics. 2013. V.138. N3. P.034706. DOI: 10.1063/1.4774375 WOS Scopus РИНЦ CAPlusCA OpenAlex
Даты:
| Поступила в редакцию: | 6 окт. 2012 г. |
| Принята к публикации: | 12 дек. 2012 г. |
| Опубликована online: | 17 янв. 2013 г. |
| Опубликована в печати: | 21 янв. 2013 г. |
Идентификаторы БД:
| Web of science: | WOS:000313671700033 |
| Scopus: | 2-s2.0-84872818581 |
| РИНЦ: | 20423201 |
| Chemical Abstracts: | 2013:97838 |
| Chemical Abstracts (print): | 158:254715 |
| OpenAlex: | W2093770411 |