Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 1, Pages 442-452Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c11752
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Funding
- National Natural Science Foundation of China [22025503, 21790361, 21871084, 21672060]
- Shanghai Municipal Science and Technology Major Project [2018SHZDZX03]
- Fundamental Research Funds for the Central Universities
- Programme of Introducing Talents of Discipline to Universities [B16017]
- Program of Shanghai Academic/Technology Research Leader [19XD1421100]
- Shanghai Science and Technology Committee [17520750100]
- Netherlands Ministry of Education, Culture and Science [024.601035]
- European Research Council (ERC) [694345]
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The study presents a visible-light-responsive molecular motor metallacycle that enables directional self-assembly of motor units through metal coordination. These metallacycles not only retain the rotation characteristics of the motors but also construct multi-component hierarchical systems, offering prospects for cooperative operations and adaptive materials.
The organization of molecular motors in supramolecular assemblies to allow the amplification and transmission of motion and collective action is an important step toward future responsive systems. Metal-coordination-driven directional self-assembly into supramolecular metallacycles provides a powerful strategy to position several motor units in larger structures with well-defined geometries. Herein, we present a pyridyl-modified molecular motor ligand (MPY) which upon coordination with geometrically distinct di-Pt(II) acceptors assembles into discrete metallacycles of different sizes and shapes. This coordination leads to a red-shift of the absorption bands of molecular motors, making these motorized metallacycles responsive to visible light. Photochemical and thermal isomerization experiments demonstrated that the light-driven rotation of the motors in the metallacycles is similar to that in free MPY in solution. CD studies show that the helicity inversions associated with each isomerization step in the rotary cycle are preserved. To explore collective motion, the trimeric motor-containing metallacycle was aggregated with heparin through multiple electrostatic interactions, to construct a multi-component hierarchical system. SEM, TEM, and DLS measurements revealed that the photo- and thermal-responsive molecular motor units enabled selective manipulation of the secondary supramolecular aggregation process without dissociating the primary metallacycle structures. These visible-light-responsive metallacycles, with intrinsic multiple rotary motors, offer prospects for cooperative operations, dynamic hierarchical self-assembled systems, and adaptive materials.
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