Spatio-Chemical Heterogeneity of Defect-Engineered Metal-Organic Framework Crystals Revealed by Full-Field Tomographic X-ray Absorption Spectroscopy.

Composite materials HKUST-1 X-ray absorption spectroscopy X-ray tomography defect engineering

Journal

Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
Titre abrégé: Angew Chem Int Ed Engl
Pays: Germany
ID NLM: 0370543

Informations de publication

Date de publication:
26 Apr 2021
Historique:
revised: 28 01 2021
received: 05 10 2020
pubmed: 2 2 2021
medline: 2 2 2021
entrez: 1 2 2021
Statut: ppublish

Résumé

The introduction of structural defects in metal-organic frameworks (MOFs), often achieved through the fractional use of defective linkers, is emerging as a means to refine the properties of existing MOFs. These linkers, missing coordination fragments, create unsaturated framework nodes that may alter the properties of the MOF. A property-targeted utilization of this approach demands an understanding of the structure of the defect-engineered MOF. We demonstrate that full-field X-ray absorption near-edge structure computed tomography can help to improve our understanding. This was demonstrated by visualizing the chemical heterogeneity found in defect-engineered HKUST-1 MOF crystals. A non-uniform incorporation and zonation of the defective linker was discovered, leading to the presence of clusters of a second coordination polymer within HKUST-1. The former is suggested to be responsible, in part, for altered MOF properties; thereby, advocating for a spatio-chemically resolved characterization of MOFs.

Identifiants

pubmed: 33523530
doi: 10.1002/anie.202013422
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

10032-10039

Subventions

Organisme : Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
ID : PZ00P2_179886

Informations de copyright

© 2021 Wiley-VCH GmbH.

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Auteurs

Dario Ferreira Sanchez (D)

Swiss Light Source, Paul Scherrer Institut (PSI), 5232, Villigen, Switzerland.

Johannes Ihli (J)

Swiss Light Source, Paul Scherrer Institut (PSI), 5232, Villigen, Switzerland.

Damin Zhang (D)

Laboratory for Catalysis and Sustainable Chemistry, Paul Scherrer Institute, 5232, Villigen PSI, Switzerland.
NanoElectroCatalysis Group, Department of Chemistry and Biochemistry, University of Bern, Bern, Switzerland.

Thomas Rohrbach (T)

Laboratory for Catalysis and Sustainable Chemistry, Paul Scherrer Institute, 5232, Villigen PSI, Switzerland.

Patric Zimmermann (P)

Laboratory for Catalysis and Sustainable Chemistry, Paul Scherrer Institute, 5232, Villigen PSI, Switzerland.

Jinhee Lee (J)

Laboratory for Catalysis and Sustainable Chemistry, Paul Scherrer Institute, 5232, Villigen PSI, Switzerland.

Camelia N Borca (CN)

Swiss Light Source, Paul Scherrer Institut (PSI), 5232, Villigen, Switzerland.

Natascha Böhlen (N)

Laboratory for Catalysis and Sustainable Chemistry, Paul Scherrer Institute, 5232, Villigen PSI, Switzerland.

Daniel Grolimund (D)

Swiss Light Source, Paul Scherrer Institut (PSI), 5232, Villigen, Switzerland.

Jeroen A van Bokhoven (JA)

Laboratory for Catalysis and Sustainable Chemistry, Paul Scherrer Institute, 5232, Villigen PSI, Switzerland.
Institute for Chemical and Bioengineering, ETH Zurich, 8093, Zürich, Switzerland.

Marco Ranocchiari (M)

Laboratory for Catalysis and Sustainable Chemistry, Paul Scherrer Institute, 5232, Villigen PSI, Switzerland.

Classifications MeSH