Chemical Feedback in Templated Reaction-Assembly Networks

Inge Bos, Camilla Terenzi, Joris Sprakel*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

4 Citations (Scopus)

Abstract

Chemical feedback between building block synthesis and their subsequent supramolecular self-assembly into nanostructures has profound effects on assembly pathways. Nature harnesses feedback in reaction-assembly networks in a variety of scenarios including virion formation and protein folding. Also in nanomaterial synthesis, reaction-assembly networks have emerged as a promising control strategy to regulate assembly processes. Yet, how chemical feedback affects the fundamental pathways of structure formation remains unclear. Here, we unravel the pathways of a templated reaction-assembly network that couples a covalent polymerization to an electrostatic coassembly process. We show how the supramolecular staging of building blocks at a macromolecular template can accelerate the polymerization reaction and prevent the formation of kinetically trapped structures inherent to the process in the absence of feedback. Finally, we establish a predictive kinetic reaction model that quantitatively describes the pathways underlying these reaction-assembly networks. Our results shed light on the fundamental mechanisms by which chemical feedback can steer self-assembly reactions and can be used to rationally design new nanostructures.

Original languageEnglish
Pages (from-to)10675-10685
Number of pages11
JournalMacromolecules
Volume53
Issue number23
DOIs
Publication statusPublished - 23 Nov 2020

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