Abstract
Supramolecular chaperones play an important role in directing the assembly of multiple protein subunits and redox-active metal ions into precise, complex and functional quaternary structures. Here we report that hydroxyl tailed C-alkylpyrogallol[4]arene ligands and redox-active MnII ions, with the assistance of proline chaperone molecules, can assemble into two-dimensional (2D) and/or three-dimensional (3D) networked nanocapsules. Dimensionality is controlled by coordination between the exterior of nanocapsule subunits, and endohedral functionalization within the 2D system is achieved via chaperone guest encapsulation. The tailoring of surface properties of nanocapsules via coordination chemistry is also shown as an effective method for the fine-tuning magnetic properties, and electrochemical and spectroscopic studies support that the nanocapsule is an effective homogeneous water-oxidation electrocatalyst, operating at pH 6.07 with an exceptionally low overpotential of 368 mV.
Highlights
Hierarchical self-assembly via metal coordination is a ubiquitous process for constructing sophisticated supramolecular structures in nature.[1]
We propose a system in which PgC3OH is assembled into hexameric hydrogen-bonded nanocapsules (MONCs), whilst proline molecules act as the molecular chaperones to capture, protect and insert the MnII ions into the framework (Scheme 1)
The crystal structure of 1 shows a 2D framework constructed from in nite metal–organic nanocapsules (MONCs) subunits, with each MONC being assembled from 30 components: six PgC3OH molecules and 24 metal ions (Fig. 1)
Summary
Hierarchical self-assembly via metal coordination is a ubiquitous process for constructing sophisticated supramolecular structures in nature.[1]. Supramolecular chaperones play an important role in directing the assembly of multiple protein subunits and redox-active metal ions into precise, complex and functional quaternary structures.
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