Charting the Metal-Dependent High-Pressure Stability of Bimetallic UiO-66 Materials.


Journal

ACS materials letters
ISSN: 2639-4979
Titre abrégé: ACS Mater Lett
Pays: United States
ID NLM: 101747116

Informations de publication

Date de publication:
06 Apr 2020
Historique:
received: 06 02 2020
accepted: 20 03 2020
entrez: 17 4 2020
pubmed: 17 4 2020
medline: 17 4 2020
Statut: ppublish

Résumé

In theory, bimetallic UiO-66(Zr:Ce) and UiO-66(Zr:Hf) metal-organic frameworks (MOFs) are extremely versatile and attractive nanoporous materials as they combine the high catalytic activity of UiO-66(Ce) or UiO-66(Hf) with the outstanding stability of UiO-66(Zr). Using in situ high-pressure powder X-ray diffraction, however, we observe that this expected mechanical stability is not achieved when incorporating cerium or hafnium in UiO-66(Zr). This observation is akin to the earlier observed reduced thermal stability of UiO-66(Zr:Ce) compounds. To elucidate the atomic origin of this phenomenon, we chart the loss-of-crystallinity pressures of 22 monometallic and bimetallic UiO-66 materials and systematically isolate their intrinsic mechanical stability from their defect-induced weakening. This complementary experimental/computational approach reveals that the intrinsic mechanical stability of these bimetallic MOFs decreases nonlinearly upon cerium incorporation but remains unaffected by the zirconium: hafnium ratio. Additionally, all experimental samples suffer from defect-induced weakening, a synthesis-controlled effect that is observed to be independent of their intrinsic stability.

Identifiants

pubmed: 32296781
doi: 10.1021/acsmaterialslett.0c00042
pmc: PMC7147928
doi:

Types de publication

Journal Article

Langues

eng

Pagination

438-445

Informations de copyright

Copyright © 2020 American Chemical Society.

Déclaration de conflit d'intérêts

The authors declare no competing financial interest.

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Auteurs

Sven M J Rogge (SMJ)

Center for Molecular Modeling (CMM), Ghent University, Technologiepark 46, B-9052 Zwijnaarde, Belgium.

Pascal G Yot (PG)

Institut Charles Gerhardt Montpellier (ICGM), Université de Montpellier, CNRS, ENSCM, Place Eugène Bataillon, F-34095 Montpellier cedex 05, France.

Jannick Jacobsen (J)

Institut für Anorganische Chemie, Christian-Albrechts-Universität zu Kiel, Max-Eyth-Straβe 2, D-24118 Kiel, Germany.

Francesco Muniz-Miranda (F)

Center for Molecular Modeling (CMM), Ghent University, Technologiepark 46, B-9052 Zwijnaarde, Belgium.

Steven Vandenbrande (S)

Center for Molecular Modeling (CMM), Ghent University, Technologiepark 46, B-9052 Zwijnaarde, Belgium.

Jonas Gosch (J)

Institut für Anorganische Chemie, Christian-Albrechts-Universität zu Kiel, Max-Eyth-Straβe 2, D-24118 Kiel, Germany.

Vanessa Ortiz (V)

Institut Charles Gerhardt Montpellier (ICGM), Université de Montpellier, CNRS, ENSCM, Place Eugène Bataillon, F-34095 Montpellier cedex 05, France.

Ines E Collings (IE)

European Synchrotron Radiation Facility, 71 Avenue des Martys, F-38000 Grenoble, France.

Sabine Devautour-Vinot (S)

Institut Charles Gerhardt Montpellier (ICGM), Université de Montpellier, CNRS, ENSCM, Place Eugène Bataillon, F-34095 Montpellier cedex 05, France.

Guillaume Maurin (G)

Institut Charles Gerhardt Montpellier (ICGM), Université de Montpellier, CNRS, ENSCM, Place Eugène Bataillon, F-34095 Montpellier cedex 05, France.

Norbert Stock (N)

Institut für Anorganische Chemie, Christian-Albrechts-Universität zu Kiel, Max-Eyth-Straβe 2, D-24118 Kiel, Germany.

Veronique Van Speybroeck (V)

Center for Molecular Modeling (CMM), Ghent University, Technologiepark 46, B-9052 Zwijnaarde, Belgium.

Classifications MeSH