Pumping between phases with a pulsed-fuel molecular ratchet
| Autor: | Ulvi Karaca, Dean Thomas, David A. Leigh, Salma Kassem, Daniel J. Tetlow, Yansong Ren |
|---|---|
| Jazyk: | angličtina |
| Předmět: |
Materials science
Polymers Ratchet Biomedical Engineering Bioengineering 010402 general chemistry 01 natural sciences Catalysis chemistry.chemical_compound General Materials Science Electrical and Electronic Engineering chemistry.chemical_classification 010405 organic chemistry Brownian ratchet Substrate (chemistry) Sorption Polymer Condensed Matter Physics Molecular machine Atomic and Molecular Physics and Optics 0104 chemical sciences Dilution chemistry Chemical engineering 13. Climate action Nanoparticles Polystyrene |
| Zdroj: | Nature Nanotechnology Thomas, D, Tetlow, D J, Ren, Y, Kassem, S, Karaca, U & Leigh, D A 2022, ' Pumping between phases with a pulsed-fuel molecular ratchet ', Nature Nanotechnology . https://doi.org/10.1038/s41565-022-01097-1 |
| ISSN: | 1748-3395 1748-3387 |
| DOI: | 10.1038/s41565-022-01097-1 |
| Popis: | The sorption of species from solution into and onto solids, surfaces, crystals, gels and other matrices, underpins the sequestering of waste and pollutants, the recovery of precious metals, heterogeneous catalysis, many forms of chemical and biological analysis and separation science, and numerous other technologies. In such cases the transfer of the substrate between phases tends to proceed spontaneously, in the direction of equilibrium. Molecular ratchet mechanisms, where kinetic gating selectively inhibits or accelerates particular steps in a process, makes it possible to drive dynamic systems out of equilibrium. Here we report on a small-molecule pump immobilised on and near the surface of polymer beads, that uses an energy ratchet mechanism to actively transport substrates from solution onto the beads away from equilibrium. One complete cycle of the pump occurs with each pulse of a chemical fuel, synchronizing the ratchet dynamics so that the immobilised molecular machines all act in unison. Upon addition of the trichloroacetic acid fuel, micrometre-diameter polystyrene beads functionalised with an average of ~8×10exp10 molecular pumps per bead, sequester from solution crown ethers appended with a fluorescent tag. Following consumption of the fuel, the rings are mechanically trapped in a higher energy, out-of-equilibrium, state on the beads and cannot be removed by dilution nor by switching the binding interactions off. This differs from dissipative assembled materials that require a continuous supply of energy to persist. Addition of a second pulse of fuel causes the uptake of more macrocycles, which can be labelled with a different fluorescent tag. This drives the system progressively further away from equilibrium and also confers sequence information on the deposited structure. The polymer-bound substrates (and the stored energy) can subsequently be released back to the bulk on demand, either emptying one compartment at a time or all at once. Non-equilibrium sorption by using immobilised artificial molecular machines to pump substrates from solution onto and into materials, offers potential for the transduction of energy from chemical fuels for the storage and release of energy and information. |
| Databáze: | OpenAIRE |
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