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http://dx.doi.org/10.18419/opus-14590
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DC Element | Wert | Sprache |
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dc.contributor.author | Grunenberg, Lars | - |
dc.contributor.author | Keßler, Christopher | - |
dc.contributor.author | Teh, Tiong Wei | - |
dc.contributor.author | Schuldt, Robin | - |
dc.contributor.author | Heck, Fabian | - |
dc.contributor.author | Kästner, Johannes | - |
dc.contributor.author | Groß, Joachim | - |
dc.contributor.author | Hansen, Niels | - |
dc.contributor.author | Lotsch, Bettina V. | - |
dc.date.accessioned | 2024-07-05T11:51:42Z | - |
dc.date.available | 2024-07-05T11:51:42Z | - |
dc.date.issued | 2024 | de |
dc.identifier.issn | 1936-086X | - |
dc.identifier.issn | 1936-0851 | - |
dc.identifier.other | 1894719174 | - |
dc.identifier.uri | http://nbn-resolving.de/urn:nbn:de:bsz:93-opus-ds-146096 | de |
dc.identifier.uri | http://elib.uni-stuttgart.de/handle/11682/14609 | - |
dc.identifier.uri | http://dx.doi.org/10.18419/opus-14590 | - |
dc.description.abstract | Covalent organic frameworks (COFs) are a class of porous materials whose sorption properties have so far been studied primarily by physisorption. Quantifying the self-diffusion of guest molecules inside their nanometer-sized pores allows for a better understanding of confinement effects or transport limitations and is thus essential for various applications ranging from molecular separation to catalysis. Using a combination of pulsed field gradient nuclear magnetic resonance measurements and molecular dynamics simulations, we have studied the self-diffusion of acetonitrile and chloroform in the 1D pore channels of two imine-linked COFs (PI-3-COF) with different levels of crystallinity and porosity. The higher crystallinity and porosity sample exhibited anisotropic diffusion for MeCN parallel to the pore direction, with a diffusion coefficient of Dpar = 6.1(3) × 10-10 m2 s-1 at 300 K, indicating 1D transport and a 7.4-fold reduction in self-diffusion compared to the bulk liquid. This finding aligns with molecular dynamics simulations predicting 5.4-fold reduction, assuming an offset-stacked COF layer arrangement. In the low-porosity sample, more frequent diffusion barriers result in isotropic, yet significantly reduced diffusivities (DB = 1.4(1) × 10-11 m2 s-1). Diffusion coefficients for chloroform at 300 K in the pores of the high- (Dpar = 1.1(2) × 10-10 m2 s-1) and low-porosity (DB = 4.5(1) × 10-12 m2 s-1) samples reproduce these trends. Our multimodal study thus highlights the significant influence of real structure effects such as stacking faults and grain boundaries on the long-range diffusivity of molecular guest species while suggesting efficient intracrystalline transport at short diffusion times. | en |
dc.description.sponsorship | Deutsche Forschungsgemeinschaft | de |
dc.description.sponsorship | Max-Planck-Gesellschaft | de |
dc.description.sponsorship | Stuttgart Center for Simulation Science | de |
dc.language.iso | en | de |
dc.relation.uri | doi:10.1021/acsnano.3c12167 | de |
dc.rights | info:eu-repo/semantics/openAccess | de |
dc.rights.uri | https://creativecommons.org/licenses/by/4.0/ | de |
dc.subject.ddc | 540 | de |
dc.title | Probing self-diffusion of guest molecules in a covalent organic framework : simulation and experiment | en |
dc.type | article | de |
dc.date.updated | 2024-06-27T03:02:58Z | - |
ubs.fakultaet | Chemie | de |
ubs.fakultaet | Energie-, Verfahrens- und Biotechnik | de |
ubs.fakultaet | Externe wissenschaftliche Einrichtungen | de |
ubs.fakultaet | Fakultätsübergreifend / Sonstige Einrichtung | de |
ubs.institut | Institut für Theoretische Chemie | de |
ubs.institut | Institut für Technische Thermodynamik und Thermische Verfahrenstechnik | de |
ubs.institut | Max-Planck-Institut für Festkörperforschung | de |
ubs.institut | Fakultätsübergreifend / Sonstige Einrichtung | de |
ubs.publikation.seiten | 16091-16100 | de |
ubs.publikation.source | ACS nano 18 (2024), S. 16091-16100 | de |
ubs.publikation.typ | Zeitschriftenartikel | de |
Enthalten in den Sammlungen: | 04 Fakultät Energie-, Verfahrens- und Biotechnik |
Dateien zu dieser Ressource:
Datei | Beschreibung | Größe | Format | |
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nn3c12167.pdf | 3,33 MB | Adobe PDF | Öffnen/Anzeigen |
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