lnu.sePublications
Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Activated Self-Resolution and Error-Correction in Catalytic Reaction Networks
KTH Royal instute of technology, Sweden.
Linnaeus University, Faculty of Health and Life Sciences, Department of Chemistry and Biomedical Sciences. KTH Royal instute of technology, Sweden;Univ Massachusetts, USA. (Linnaeus Ctr Biomat Chem, BMC;BBCL)ORCID iD: 0000-0002-1533-6514
2021 (English)In: Chemistry - A European Journal, ISSN 0947-6539, E-ISSN 1521-3765, Vol. 27, no 40, p. 10335-10340Article in journal (Refereed) Published
Abstract [en]

Understanding the emergence of function in complex reaction networks is a primary goal of systems chemistry and origin-of-life studies. Especially challenging is to create systems that simultaneously exhibit several emergent functions that can be independently tuned. In this work, a multifunctional complex reaction network of nucleophilic small molecule catalysts for the Morita-Baylis-Hillman (MBH) reaction is demonstrated. The dynamic system exhibited triggered self-resolution, preferentially amplifying a specific catalyst/product set out of a many potential alternatives. By utilizing selective reversibility of the products of the reaction set, systemic thermodynamically driven error-correction could also be introduced. To achieve this, a dynamic covalent MBH reaction based on adducts with internal H-transfer capabilities was developed. By careful tuning of the substituents, rate accelerations of retro-MBH reactions of up to four orders of magnitude could be obtained. This study thus demonstrates how efficient self-sorting of catalytic systems can be achieved through an interplay of several complex emergent functionalities.

Place, publisher, year, edition, pages
John Wiley & Sons, 2021. Vol. 27, no 40, p. 10335-10340
Keywords [en]
dynamic covalent chemistry, dynamic systems, imine exchange, Morita-Baylis-Hillman reactions, organocatalysis
National Category
Organic Chemistry
Research subject
Chemistry, Organic Chemistry
Identifiers
URN: urn:nbn:se:lnu:diva-103700DOI: 10.1002/chem.202100208ISI: 000645519500001PubMedID: 33780566Scopus ID: 2-s2.0-85105174812Local ID: 2021OAI: oai:DiVA.org:lnu-103700DiVA, id: diva2:1559537
Note

A previous version of this manuscript has been deposited on a preprint server: https://doi.org/10.26434/chemrxiv.13604318.v1

Available from: 2021-06-02 Created: 2021-06-02 Last updated: 2022-03-15Bibliographically approved

Open Access in DiVA

No full text in DiVA

Other links

Publisher's full textPubMedScopusSupporting information

Authority records

Ramström, Olof

Search in DiVA

By author/editor
Ramström, Olof
By organisation
Department of Chemistry and Biomedical Sciences
In the same journal
Chemistry - A European Journal
Organic Chemistry

Search outside of DiVA

GoogleGoogle Scholar

doi
pubmed
urn-nbn

Altmetric score

doi
pubmed
urn-nbn
Total: 46 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf