Nonstatistical assembly of multicomponent [Pd2ABCD] cages
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Date
2024-01-19
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Abstract
Self-assembled hosts, inspired by biological receptors and catalysts, show
potential for sustainable synthesis, energy conversion and medicine. Implementing multiple
functionalities in the form of distinguishable building blocks, however, is difficult without
risking narcissistic self-sorting or statistical mess. Here, we report a systematic series of
integratively self-assembled heteroleptic cages in which two square-planar PdII cations are
bridged by four different bis-pyridyl ligands A, B, C and D via synergistic effects to exclusively
form a single isomer — the lantern-shaped cage [Pd2ABCD]. This self-sorting goal — forming
just one out of 55 possible structures — is reached under full thermodynamic control and can
be realized progressively (by combining progenitors such as [Pd2A2C2] with [Pd2B2D2]),
directly from ligands and PdII cations, or by mixing all four corresponding homoleptic cages.
The rational design of complex multicomponent assemblies that enables the incorporation of
chemical moieties in a modular approach will advance their potential applications in functional
nanosystems.
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Keywords
coordination cages, supramolecular chemistry, self sorting