Noncovalent synthesis of homo and hetero-architectures of supramolecular polymers via secondary nucleation

Srinu Kotha, Rahul Sahu, Aditya Chandrakant Yadav, Preeti Sharma, B. V. V. S. Pavan Kumar, Sandeep K. Reddy () and Kotagiri Venkata Rao ()
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Srinu Kotha: Indian Institute of Technology Hyderabad, Kandi
Rahul Sahu: Indian Institute of Technology Kharagpur
Aditya Chandrakant Yadav: Indian Institute of Technology Hyderabad, Kandi
Preeti Sharma: Indian Institute of Technology
B. V. V. S. Pavan Kumar: Indian Institute of Technology
Sandeep K. Reddy: Indian Institute of Technology Kharagpur
Kotagiri Venkata Rao: Indian Institute of Technology Hyderabad, Kandi

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract The synthesis of supramolecular polymers with controlled architecture is a grand challenge in supramolecular chemistry. Although living supramolecular polymerization via primary nucleation has been extensively studied for controlling the supramolecular polymerization of small molecules, the resulting supramolecular polymers have typically exhibited one-dimensional morphology. In this report, we present the synthesis of intriguing supramolecular polymer architectures through a secondary nucleation event, a mechanism well-established in protein aggregation and the crystallization of small molecules. To achieve this, we choose perylene diimide with 2-ethylhexyl chains at the imide position as they are capable of forming dormant monomers in solution. Activating these dormant monomers via mechanical stimuli and hetero-seeding using propoxyethyl perylene diimide seeds, secondary nucleation event takes over, leading to the formation of three-dimensional spherical spherulites and scarf-like supramolecular polymer heterostructures, respectively. Therefore, the results presented in this study propose a simple molecular design for synthesizing well-defined supramolecular polymer architectures via secondary nucleation.

Date: 2024
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DOI: 10.1038/s41467-024-47874-5

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