Controlled self‐assembly of cage‐like structures and their applications in fullerene chemistry
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Date
2019
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Abstract
This thesis showcases the donor-site engineering in PdII-mediated coordination complexes, yielding distinctive supramolecular architectures, including the molecular cage, bowl, ring and capsule focuses on the donor-site-controlled self-assembly of supramolecules as well as their distinct fullerene binding abilities. Afterwards, the assembled cage is able to selectively bind C60 from fullerene soot, and develops into a recyclable system of C60 purification controlled by solvent effects. The novel bowl structure is not only found to serve as a supramolecular protecting group, which allows selective mono-functionalization of its guest, but is also capable of being connected by a second ligand to hierarchically assemble into a molecular capsule which can accommodate two fullerene molecules within its inner cavity. In addition, a non-traditional nitrogen donor, namely naphthyridine, is shown to manifest a dislocated arrangement in the PdII coordination sphere owing to the repulsive effect between adjacent electron-pairs. A synergy between quinoline donors and naphthyridine donors as well as template effect of guests is further exploited to generate heteroleptic cages. At last, a newly designed fullerene-based ligand can assemble with PdII into a coordination cage bearing four fullerene molecules in the periphery. All compounds have been fully characterized by multiple analytic techniques, such as NMR spectroscopy, mass spectrometry and single crystal X-ray structural analysis.
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Supramolecular chemistry, Self-assembly, Coordination cage, Fullerene, Functionalization, Fullerene separation
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Supramolekulare Chemie, Selbstorganisation, Koordinationsverbindungen