Membrane transport modulates the pH-regulated feedback of an enzyme reaction confined within lipid vesicles
Membrane transport modulates the pH-regulated feedback of an enzyme reaction confined within lipid vesicles
Understanding ion transport dynamics in reactive vesicles is pivotal for exploring biological and chemical processes and essential for designing synthetic cells. In this work, we investigate how proton transport and membrane potential regulate pH dynamics in an autocatalytic enzyme reaction within lipid vesicles. Combining experimental and numerical methods, we demonstrate that compartmentalization within lipid membranes accelerates internal reactions, attributed to protection from the external acidic environment. In experiments, we explored how proton movement significantly impacts internal reactions by changing bilayer thickness, adding ion transporters, and varying buffers. Numerical investigations incorporated electrical membrane potential and capacitance into a kinetic model of the process, elucidating the mechanisms that dictate the control of reaction time observed in the experiment, driven by both electrical and chemical potential gradients. These findings establish a framework for controlling pH clock reactions via membrane changes and targeted manipulation of proton movement, which could aid in the design of synthetic cells with precise, controlled functionalities.
confinement, enzymes, membrane, pH, permeability, urease, vesicles
9814-9825
Ridgway-Brown, Darcey
58228dd3-75a1-4bd3-9ab3-8555b0a564c3
Leathard, Anna S.
82fc63a9-7d0c-483b-9770-da084719e40d
France, Oliver
d6806568-4d46-4cf8-979e-37811a9b64ea
Muench, Stephen P.
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Webb, Michael E.
e0e98c04-cfbf-4e56-be1f-e88966bca635
Jeuken, Lars J.C.
ba3d8fad-754e-4521-b86e-7f4f468893e4
Henderson, Peter J. F.
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Taylor, Annette F.
08028a29-428d-4732-b6b1-f7a93389b386
Beales, Paul A.
920bef12-e354-4ff6-a528-9cab2227f32e
18 March 2025
Ridgway-Brown, Darcey
58228dd3-75a1-4bd3-9ab3-8555b0a564c3
Leathard, Anna S.
82fc63a9-7d0c-483b-9770-da084719e40d
France, Oliver
d6806568-4d46-4cf8-979e-37811a9b64ea
Muench, Stephen P.
4ba445ee-0fee-4f85-b206-89093f00abba
Webb, Michael E.
e0e98c04-cfbf-4e56-be1f-e88966bca635
Jeuken, Lars J.C.
ba3d8fad-754e-4521-b86e-7f4f468893e4
Henderson, Peter J. F.
5f8b6617-59b9-4c35-99db-a5733516610b
Taylor, Annette F.
08028a29-428d-4732-b6b1-f7a93389b386
Beales, Paul A.
920bef12-e354-4ff6-a528-9cab2227f32e
Ridgway-Brown, Darcey, Leathard, Anna S., France, Oliver, Muench, Stephen P., Webb, Michael E., Jeuken, Lars J.C., Henderson, Peter J. F., Taylor, Annette F. and Beales, Paul A.
(2025)
Membrane transport modulates the pH-regulated feedback of an enzyme reaction confined within lipid vesicles.
ACS Nano, 19 (10), .
(doi:10.1021/acsnano.4c13048).
Abstract
Understanding ion transport dynamics in reactive vesicles is pivotal for exploring biological and chemical processes and essential for designing synthetic cells. In this work, we investigate how proton transport and membrane potential regulate pH dynamics in an autocatalytic enzyme reaction within lipid vesicles. Combining experimental and numerical methods, we demonstrate that compartmentalization within lipid membranes accelerates internal reactions, attributed to protection from the external acidic environment. In experiments, we explored how proton movement significantly impacts internal reactions by changing bilayer thickness, adding ion transporters, and varying buffers. Numerical investigations incorporated electrical membrane potential and capacitance into a kinetic model of the process, elucidating the mechanisms that dictate the control of reaction time observed in the experiment, driven by both electrical and chemical potential gradients. These findings establish a framework for controlling pH clock reactions via membrane changes and targeted manipulation of proton movement, which could aid in the design of synthetic cells with precise, controlled functionalities.
Text
ridgway-brown-et-al-2025-membrane-transport-modulates-the-ph-regulated-feedback-of-an-enzyme-reaction-confined-within
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Accepted/In Press date: 21 February 2025
Published date: 18 March 2025
Keywords:
confinement, enzymes, membrane, pH, permeability, urease, vesicles
Identifiers
Local EPrints ID: 500102
URI: http://eprints.soton.ac.uk/id/eprint/500102
ISSN: 1936-0851
PURE UUID: 0c550b15-6513-49c3-8d54-13d9d1394dd4
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Date deposited: 15 Apr 2025 16:58
Last modified: 22 Aug 2025 02:44
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Contributors
Author:
Darcey Ridgway-Brown
Author:
Anna S. Leathard
Author:
Oliver France
Author:
Stephen P. Muench
Author:
Michael E. Webb
Author:
Lars J.C. Jeuken
Author:
Peter J. F. Henderson
Author:
Annette F. Taylor
Author:
Paul A. Beales
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