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.

Dissipative catalysis with a molecular machine / Biagini, C.; Fielden, S. D. P.; Leigh, D. A.; Schaufelberger, F.; DI STEFANO, Stefano; Thomas, D.. - In: ANGEWANDTE CHEMIE. INTERNATIONAL EDITION. - ISSN 1433-7851. - 58:29(2019), pp. 9876-9880. [10.1002/anie.201905250]

Dissipative catalysis with a molecular machine

Biagini C.;Di Stefano S.;
2019

Abstract

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.
2019
chemical fuels; hydrogen-bonding catalysis; molecular machines; out-of-equilibrium systems; rotaxanes
01 Pubblicazione su rivista::01a Articolo in rivista
Dissipative catalysis with a molecular machine / Biagini, C.; Fielden, S. D. P.; Leigh, D. A.; Schaufelberger, F.; DI STEFANO, Stefano; Thomas, D.. - In: ANGEWANDTE CHEMIE. INTERNATIONAL EDITION. - ISSN 1433-7851. - 58:29(2019), pp. 9876-9880. [10.1002/anie.201905250]
File allegati a questo prodotto
File Dimensione Formato  
Biagini_Dissipative_2019.pdf

accesso aperto

Tipologia: Versione editoriale (versione pubblicata con il layout dell'editore)
Licenza: Creative commons
Dimensione 2.39 MB
Formato Adobe PDF
2.39 MB Adobe PDF

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11573/1305582
Citazioni
  • ???jsp.display-item.citation.pmc??? 17
  • Scopus 101
  • ???jsp.display-item.citation.isi??? 98
social impact