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Dissipative Catalysis with a Molecular Machine.

Chiara Biagini1,2, Stephen D P Fielden1, David A Leigh1

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Summary
This summary is machine-generated.

Synthetic molecular machines can be switched between active and inactive states using fuel pulses. This controlled catalysis enables temporal regulation, paving the way for advanced molecular networks.

Keywords:
chemical fuelshydrogen-bonding catalysismolecular machinesout-of-equilibrium systemsrotaxanes

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Area of Science:

  • Supramolecular Chemistry
  • Catalysis
  • Molecular Machines

Background:

  • Synthetic molecular machines offer precise control over chemical processes.
  • Transient states in molecular systems are crucial for dynamic functions.
  • Fuel-induced switching is a key mechanism for activating molecular devices.

Purpose of the Study:

  • To investigate fuel-induced transient states for catalysis in a synthetic molecular machine.
  • To achieve temporal control over catalytic activity using chemical fuel pulses.
  • To explore the design principles for dissipative catalysis in molecular networks.

Main Methods:

  • Utilized a [2]rotaxane molecular shuttle with ammonium/amine and thiourea stations.
  • Activated and deactivated the rotaxane's catalytic state using pulses of trichloroacetic acid fuel.
  • Quantified catalytic activity via transfer hydrogenation of nitrostyrene.
  • Regulated the duration of the catalytic ON-state by varying fuel concentration.

Main Results:

  • The molecular shuttle transitions between catalytically inactive and active states.
  • The active state catalyzes nitrostyrene reduction through transfer hydrogenation.
  • The lifetime of the catalytic state is precisely controlled by the amount of fuel added.
  • The system demonstrated repeated, pulsed activation of catalysis.

Conclusions:

  • Fuel-induced transient states enable temporal control of synthetic molecular machine catalysis.
  • Dissipative catalysis in molecular machines is achievable and tunable.
  • This work has implications for designing responsive molecular networks with signaling capabilities.