Towards general network architecture design criteria for negative gas adsorption transitions in ultraporous frameworks.


Journal

Nature communications
ISSN: 2041-1723
Titre abrégé: Nat Commun
Pays: England
ID NLM: 101528555

Informations de publication

Date de publication:
12 Aug 2019
Historique:
received: 19 03 2019
accepted: 23 07 2019
entrez: 14 8 2019
pubmed: 14 8 2019
medline: 14 8 2019
Statut: epublish

Résumé

Switchable metal-organic frameworks (MOFs) have been proposed for various energy-related storage and separation applications, but the mechanistic understanding of adsorption-induced switching transitions is still at an early stage. Here we report critical design criteria for negative gas adsorption (NGA), a counterintuitive feature of pressure amplifying materials, hitherto uniquely observed in a highly porous framework compound (DUT-49). These criteria are derived by analysing the physical effects of micromechanics, pore size, interpenetration, adsorption enthalpies, and the pore filling mechanism using advanced in situ X-ray and neutron diffraction, NMR spectroscopy, and calorimetric techniques parallelised to adsorption for a series of six isoreticular networks. Aided by computational modelling, we identify DUT-50 as a new pressure amplifying material featuring distinct NGA transitions upon methane and argon adsorption. In situ neutron diffraction analysis of the methane (CD

Identifiants

pubmed: 31406113
doi: 10.1038/s41467-019-11565-3
pii: 10.1038/s41467-019-11565-3
pmc: PMC6690989
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

3632

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Auteurs

Simon Krause (S)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany.

Jack D Evans (JD)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany.
Chimie ParisTech, PSL University, CNRS, Institut de Recherche de Chimie, Paris, 75005, Paris, France.

Volodymyr Bon (V)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany.

Irena Senkovska (I)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany.

Paul Iacomi (P)

Aix-Marseille Univ., CNRS, MADIREL (UMR 7246), 13013, Marseille, France.

Felicitas Kolbe (F)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany.

Sebastian Ehrling (S)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany.

Erik Troschke (E)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany.

Jürgen Getzschmann (J)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany.

Daniel M Többens (DM)

Helmholtz-Zentrum Berlin für Materialien und Energie, Hahn-Meitner-Platz 1, 14109, Berlin, Germany.

Alexandra Franz (A)

Helmholtz-Zentrum Berlin für Materialien und Energie, Hahn-Meitner-Platz 1, 14109, Berlin, Germany.

Dirk Wallacher (D)

Helmholtz-Zentrum Berlin für Materialien und Energie, Hahn-Meitner-Platz 1, 14109, Berlin, Germany.

Pascal G Yot (PG)

Institut Charles Gerhardt Montpellier UMR 5253 Univ. Montpellier CNRS UM ENSCM, Université de Montpellier, Place Eugène Bataillon, 34095, Montpellier cedex 05, France.

Guillaume Maurin (G)

Institut Charles Gerhardt Montpellier UMR 5253 Univ. Montpellier CNRS UM ENSCM, Université de Montpellier, Place Eugène Bataillon, 34095, Montpellier cedex 05, France.

Eike Brunner (E)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany.

Philip L Llewellyn (PL)

Aix-Marseille Univ., CNRS, MADIREL (UMR 7246), 13013, Marseille, France.

François-Xavier Coudert (FX)

Chimie ParisTech, PSL University, CNRS, Institut de Recherche de Chimie, Paris, 75005, Paris, France.

Stefan Kaskel (S)

Faculty of Chemistry and Food Chemistry, TU Dresden, Bergstrasse 66, 01062, Dresden, Germany. stefan.kaskel@tu-dresden.de.

Classifications MeSH