Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 25, Issue 8, Pages 2051-2058Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201805024
Keywords
in situ PDF; metal-organic frameworks; nucleation; secondary building units; UiO-66
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Funding
- Danish National Research Foundation [DNRF93]
- National Natural Science Foundation of China [51602301]
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The concept of secondary building units (SBUs) is central to all science on metal-organic frameworks (MOFs), and they are widely used to design new MOF materials. However, the presence of SBUs during MOF formation remains controversial, and the formation mechanism of MOFs remains unclear, due to limited information about the evolution of prenucleation cluster structures. Here in situ pair distribution function (PDF) analysis was used to probe UiO-66 formation under solvothermal conditions. The expected SBUa hexanuclear zirconium clusteris present in the metal salt precursor solution. Addition of organic ligands results in a disordered structure with correlations up to 23 angstrom, resembling crystalline UiO-66. Heating leads to fast cluster aggregation, and further growth and ordering results in the crystalline product. Thus, SBUs are present already at room temperature and act as building blocks for MOF formation. The proposed formation steps provide insight for further development of MOF synthesis.
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