Journal
INORGANIC CHEMISTRY
Volume 60, Issue 12, Pages 8973-8983Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.1c00871
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Funding
- Ministry of Science and Technology Taiwan [MOST 109-2113-M-259-008]
- National Research Foundation of South Africa [132014]
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The study presents the synthesis of a solvated non-cyclic hexadecanuclear cluster and its subsequent self-assembly into a giant metallaring using a potentially heteroditopic monothiocarbonate ligand. The resulting highest nuclearity copper(I) wheel exhibits solid-state luminescence and a luminescent precursor to the cluster can be achieved through a solventless mechanochemical synthesis.
The hierarchical self-organization of structurally complex high-nuclearity metal clusters with metallosupramolecular wheel architectures that are obtained from the self-assembly of smaller solvated cluster units is rare and unique. Here, we use the potentially heteroditopic monothiocarbonate ligand and demonstrate for the first time the synthesis and structure of a solvated non-cyclic hexadecanuclear cluster [Cu{SC(O)O'Pr}](16)center dot 2THF (1) that can simultaneously desolvate and self-assemble in solution and subsequently form a giant metallaring, [Cu{SC(O)O'Pr}](96) (2). We also demonstrate a luminescent precursor to cluster (2) can be achieved through a solventless and rapid mechanochemical synthesis. Cluster (2) is the highest nuclearity copper(I) wheel and the largest metal cluster containing a heterodichalcogen (O, S) ligand reported to date. Cluster (2) also exhibits solid-state luminescence with relatively long emission lifetimes at 4.1, 13.9 (mu s). The synthetic strategy described here opens new research avenues by replacing solvent molecules in stable {Cu-16} clusters with designed building units that can form new hybrid and multifunctional finite supramolecular materials. This finding may lead to the development of novel high-nuclearity materials self-assembled in a facile manner with tunable optical properties.
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