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Sökning: WFRF:(Cliffe A.)

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  • Cliffe, Matthew J., et al. (författare)
  • Correlated defect nanoregions in a metal-organic framework
  • 2014
  • Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 5, s. 4176-
  • Tidskriftsartikel (refereegranskat)abstract
    • Throughout much of condensed matter science, correlated disorder is a key to material function. While structural and compositional defects are known to exist within a variety of metal-organic frameworks (MOFs), the prevailing understanding is that these defects are only ever included in a random manner. Here we show-using a combination of diffuse scattering, electron microscopy, anomalous X-ray scattering and pair distribution function measurements-that correlations between defects can in fact be introduced and controlled within a hafnium terephthalate MOF. The nanoscale defect structures that emerge are an analogue of correlated Schottky vacancies in rocksalt-structured transition metal monoxides and have implications for storage, transport, optical and mechanical responses. Our results suggest how the diffraction behaviour of some MOFs might be reinterpreted, and establish a strategy of exploiting correlated nanoscale disorder as a targetable and desirable motif in MOF design.
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  • Prasad, Ram R. R., et al. (författare)
  • Modulated Self-Assembly of Catalytically Active Metal-Organic Nanosheets Containing Zr6 Clusters and Dicarboxylate Ligands
  • 2024
  • Ingår i: ACS Applied Materials and Interfaces. - 1944-8244 .- 1944-8252. ; 16:14, s. 17812-17820
  • Tidskriftsartikel (refereegranskat)abstract
    • Two-dimensional metal–organic nanosheets (MONs) have emerged as attractive alternatives to their three-dimensional metal–organic framework (MOF) counterparts for heterogeneous catalysis due to their greater external surface areas and higher accessibility of catalytically active sites. Zr MONs are particularly prized because of their chemical stability and high Lewis and Brønsted acidities of the Zr clusters. Herein, we show that careful control over modulated self-assembly and exfoliation conditions allows the isolation of the first example of a two-dimensional nanosheet wherein Zr6 clusters are linked by dicarboxylate ligands. The hxl topology MOF, termed GUF-14 (GUF = Glasgow University Framework), can be exfoliated into monolayer thickness hns topology MONs, and acid-induced removal of capping modulator units yields MONs with enhanced catalytic activity toward the formation of imines and the hydrolysis of an organophosphate nerve agent mimic. The discovery of GUF-14 serves as a valuable example of the undiscovered MOF/MON structural diversity extant in established metal–ligand systems that can be accessed by harnessing the power of modulated self-assembly protocols.
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