Connecting Defects and Amorphization in UiO-66 and MIL-140 Metal-organic Frameworks: A Combined Experimental and Computational StudyReport as inadecuate


Connecting Defects and Amorphization in UiO-66 and MIL-140 Metal-organic Frameworks: A Combined Experimental and Computational Study


Connecting Defects and Amorphization in UiO-66 and MIL-140 Metal-organic Frameworks: A Combined Experimental and Computational Study - Download this document for free, or read online. Document in PDF available to download.

Publication Date: 2015-12-02

Journal Title: Physical Chemistry Chemical Physics

Publisher: Royal Society of Chemistry

Volume: 18

Pages: 2192-2201

Language: English

Type: Article

Metadata: Show full item record

Citation: Bennett, T. D., Todorova, T., Baxter, E., Reid, D. G., Gervais, C., Bueken, B., van de Voorde, B., et al. (2015). Connecting Defects and Amorphization in UiO-66 and MIL-140 Metal-organic Frameworks: A Combined Experimental and Computational Study. Physical Chemistry Chemical Physics, 18 2192-2201.

Description: This is the final version of the article. It was first available from the Royal Society of Chemistry via http://dx.doi.org/10.1039/C5CP06798G

Abstract: The mechanism and products of the structural collapse of the metal-organic frameworks (MOFs) UiO-66, MIL-140B and MIL-140C upon ball-milling are investigated through solid state 13C NMR and pair distribution function (PDF) studies, finding amorphization to proceed by the breaking of a fraction of metal-ligand bonding in each case. The amorphous products contain inorganic-organic bonding motifs reminiscent of the crystalline phases. Whilst the inorganic Zr6O4(OH)4 clusters of UiO-66 remain intact upon structural collapse, the ZrO backbone of the MIL-140 frameworks undergoes substantial distortion. Density functional theory calculations have been performed to investigate defective models of MIL-140B and show, through comparison of calculated and experimental 13C NMR spectra, that amorphization and defects in the materials are linked.

Sponsorship: The manuscript was written through contributions of all authors. TDB conceived the initial project. T.D.B. acknowledges Trinity Hall (University of Cambridge) and Professor Anthony K. Cheetham for use of lab facilities. D.G.R. acknowledges the UK MRC for financial support. The authors acknowledge Diamond Light Source for the provision of synchrotron access to Beamline I15 (ex p. EE9691) and Philip A. Chater and Andrew Cairns for assistance with data collection. T.K.T. and C.M.D. thank the French National Research Agency (ANR project: HOPFAME ANR-13-BS07-0002-01) and the Foundation de l'Orangerie for funding. The calculations have been performed using the HPC resources from GENCI (CINES/TGCC/IDRIS) through Grant (2015-097343 and -091461). B.B., B.V.d.V. and D.D.V . gratefully acknowledge the FWO for funding (aspirant grant).

Identifiers:

This record's URL: http://dx.doi.org/10.1039/C5CP06798Ghttps://www.repository.cam.ac.uk/handle/1810/252848

Rights: Creative Commons Attribution 4.0 International License

Licence URL: http://creativecommons.org/licenses/by/4.0/





Author: Bennett, Thomas DouglasTodorova, TanyaBaxter, EmmaReid, David G.Gervais, ChristelBueken, Bartvan de Voorde, BenVos, Dirk E. deKeen

Source: https://www.repository.cam.ac.uk/handle/1810/252848



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