Dissipative Catalysis with a Molecular Machine.
chemical fuels
hydrogen-bonding catalysis
molecular machines
out-of-equilibrium systems
rotaxanes
Journal
Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
Titre abrégé: Angew Chem Int Ed Engl
Pays: Germany
ID NLM: 0370543
Informations de publication
Date de publication:
15 Jul 2019
15 Jul 2019
Historique:
received:
27
04
2019
pubmed:
22
5
2019
medline:
22
5
2019
entrez:
22
5
2019
Statut:
ppublish
Résumé
We report on catalysis by a fuel-induced transient state of a synthetic molecular machine. A [2]rotaxane molecular shuttle containing secondary ammonium/amine and thiourea stations is converted between catalytically inactive and active states by pulses of a chemical fuel (trichloroacetic acid), which is itself decomposed by the machine and/or the presence of additional base. The ON-state of the rotaxane catalyzes the reduction of a nitrostyrene by transfer hydrogenation. By varying the amount of fuel added, the lifetime of the rotaxane ON-state can be regulated and temporal control of catalysis achieved. The system can be pulsed with chemical fuel several times in succession, with each pulse activating catalysis for a time period determined by the amount of fuel added. Dissipative catalysis by synthetic molecular machines has implications for the future design of networks that feature communication and signaling between the components.
Identifiants
pubmed: 31111628
doi: 10.1002/anie.201905250
pmc: PMC6900173
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
9876-9880Subventions
Organisme : EPSRC
ID : EP/P027067/1
Organisme : ERC
ID : Advanced Grant no. 786630
Organisme : Marie Skłodowska-Curie Individual Postdoctoral Fellowship
ID : EC 746993
Organisme : La Sapienza
ID : CESaRe project
Organisme : Royal Society
ID : Research Professorship
Informations de copyright
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
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