A1 Refereed original research article in a scientific journal
Mutualistic Synthesis from Orthogonal Dynamic Covalent Reactions
Authors: Lyu, Yonglei; Hu, Ying; Yang, Jinghui; Wang, Xin; Li, Jianwei
Publisher: Wiley-VCH
Publication year: 2024
Journal: Angewandte Chemie International Edition
Journal name in source: Angewandte Chemie (International ed. in English)
Journal acronym: Angew Chem Int Ed Engl
Article number: e202412020
Volume: 63
Issue: 44
ISSN: 1433-7851
eISSN: 1521-3773
DOI: https://doi.org/10.1002/anie.202412020
Web address : https://onlinelibrary.wiley.com/doi/10.1002/anie.202412020
Self-archived copy’s web address: https://research.utu.fi/converis/portal/detail/Publication/457218741
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.).