Photoswitchable gating of non-equilibrium enzymatic feedback in chemically communicating polymersome nanoreactors

Rifaie-Graham, Omar and Yeow, Jonathan and Najer, Adrian and Wang, Richard and Sun, Rujie and Zhou, Kun and Dell, Tristan N. and Adrianus, Christopher and Thanapongpibul, Chalaisorn and Chami, Mohamed and Mann, Stephen and de Alaniz, Javier Read and Stevens, Molly M.. (2022) Photoswitchable gating of non-equilibrium enzymatic feedback in chemically communicating polymersome nanoreactors. Nature Chemistry, 15 (1). pp. 110-118.

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Official URL: https://edoc.unibas.ch/90245/

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The circadian rhythm generates out-of-equilibrium metabolite oscillations that are controlled by feedback loops under light/dark cycles. Here we describe a non-equilibrium nanosystem comprising a binary population of enzyme-containing polymersomes capable of light-gated chemical communication, controllable feedback and coupling to macroscopic oscillations. The populations consist of esterase-containing polymersomes functionalized with photo-responsive donor-acceptor Stenhouse adducts (DASA) and light-insensitive semipermeable urease-loaded polymersomes. The DASA-polymersome membrane becomes permeable under green light, switching on esterase activity and decreasing the pH, which in turn initiates the production of alkali in the urease-containing population. A pH-sensitive pigment that absorbs green light when protonated provides a negative feedback loop for deactivating the DASA-polymersomes. Simultaneously, increased alkali production deprotonates the pigment, reactivating esterase activity by opening the membrane gate. We utilize light-mediated fluctuations of pH to perform non-equilibrium communication between the nanoreactors and use the feedback loops to induce work as chemomechanical swelling/deswelling oscillations in a crosslinked hydrogel. We envision possible applications in artificial organelles, protocells and soft robotics.
Faculties and Departments:05 Faculty of Science > Departement Biozentrum > Services Biozentrum > BioEM Lab (Chami)
05 Faculty of Science > Departement Biozentrum > Former Organization Units Biozentrum > Structural Biology (Engel)
05 Faculty of Science > Departement Biozentrum > Structural Biology & Biophysics > Structural Biology and Biophysics (Engel)
UniBasel Contributors:Chami, Mohamed
Item Type:Article, refereed
Article Subtype:Research Article
Note:Publication type according to Uni Basel Research Database: Journal article
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Last Modified:24 Oct 2023 13:21
Deposited On:24 Jan 2023 13:55

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