Controlled hierarchical self-assembly of networked coordination nanocapsules via the use of molecular chaperones

Xiangquan Hu; Sisi Feng; Jialei Du; Li Shao; Jinxin Lang; Chen Zhang; Steven P. Kelley; Jian Lin; Scott J. Dalgarno; David A. Atwood; Jerry L. Atwood

doi:10.1039/D0SC05002D

Controlled hierarchical self-assembly of networked coordination nanocapsules via the use of molecular chaperones†

Xiangquan Hu,^a Sisi Feng,

*^b Jialei Du,*^c Li Shao,^a Jinxin Lang,^d Chen Zhang,

^e Steven P. Kelley,^a Jian Lin,

^f Scott J. Dalgarno,

^g David A. Atwood^h and Jerry L. Atwood

*^a

Author affiliations

* Corresponding authors

^a Department of Chemistry, University of Missouri-Columbia, 601 S College Ave, Columbia, MO 65211, USA
E-mail: atwood@missouri.edu

^b Key Laboratory of Chemical Biology and Molecular Engineering of Ministry of Education, Institute of Molecular Science, Shanxi University, Taiyuan 030006, P. R. China
E-mail: ssfeng@sxu.edu.cn

^c Institute for Advanced Interdisciplinary Research, University of Jinan, Jinan 250022, P. R. China
E-mail: ifc_dujl@ujn.edu.cn

^d School of Chemistry, Xi'an Jiaotong University, Xi'an 710049, P. R. China

^e Department of Chemical and Biomolecular Engineering, North Carolina Sate University, Raleigh, North Carolina 27695, USA

^f Department of Mechanical and Aerospace Engineering, University of Missouri-Columbia, 601 S College Ave, Columbia, MO 65211, USA

^g Institute of Chemical Sciences, Heriot-Watt University, Riccarton, Edinburgh EH14 4AS, UK

^h Department of Chemistry, University of Kentucky, Lexington, KY 40506, USA

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 Mn^II ions, with the assistance of proline chaperone molecules, can assemble into two-dimensional (2D) and/or three-dimensional (3D) networked Image ID:d0sc05002d-t2.gif 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 Image ID:d0sc05002d-t3.gif nanocapsule is an effective homogeneous water-oxidation electrocatalyst, operating at pH 6.07 with an exceptionally low overpotential of 368 mV.

Chemical Science

Controlled hierarchical self-assembly of networked coordination nanocapsules via the use of molecular chaperones†

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Controlled hierarchical self-assembly of networked coordination nanocapsules via the use of molecular chaperones

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