A1 Refereed original research article in a scientific journal

Mutualistic Synthesis from Orthogonal Dynamic Covalent Reactions




AuthorsLyu, Yonglei; Hu, Ying; Yang, Jinghui; Wang, Xin; Li, Jianwei

PublisherWiley-VCH

Publication year2024

JournalAngewandte Chemie International Edition

Journal name in sourceAngewandte Chemie (International ed. in English)

Journal acronymAngew Chem Int Ed Engl

Article numbere202412020

Volume63

Issue44

ISSN1433-7851

eISSN1521-3773

DOIhttps://doi.org/10.1002/anie.202412020

Web address https://onlinelibrary.wiley.com/doi/10.1002/anie.202412020

Self-archived copy’s web addresshttps://research.utu.fi/converis/portal/detail/Publication/457218741


Abstract
Mutualisms are interactions that benefit all species involved. It has been widely investigated in neighbouring subjects, such as biology, ecology, sociology, and economics. However, such a reciprocal relationship in synthetic chemical systems has rarely been studied. Here, we demonstrate a mutualistic synthesis where byproducts from two orthogonal chemical reactions aid each other's production. Disulfide exchange and hydrazone exchange were chosen to generate two dynamic combinatorial libraries. A minor tetrameric macrocycle from the active disulfide library was quantitatively amplified in the presence of the hydrazone library. This incorporation also turned on the previously inert hydrazone reaction, producing a linear species that formed a "handcuffs" catenane with the disulfide tetramer. These findings not only lend robust support to the hypothesis of "RNA-peptide coevolution" for the origin of life but also broaden the scope of synthetic chemistry, highlighting the untapped potential of minor products from different reactions. Additionally, the co-self-assembly of these mutualistic entities to form supramolecular structures opens new avenues for future development of composite nanosystems with synergistic properties.

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Funding information in the publication
We are grateful for the financial support from the Sigrid JuséliusFoundation (senior researcher fellowship for J.L.), the Academyof Finland (Decision No.318524, project funding for J.L.), theFinnish Cultural Foundation (PhD fellowship for Y.L.) and ChinaScholarship Council (PhD scholarship for J.Y. and X.W.).


Last updated on 2025-27-01 at 18:29