A light-fuelled nanoratchet shifts a coupled chemical equilibrium

Michael Kathan*, Stefano Crespi, Niklas O Thiel, Daniel L Stares, Denis Morsa, John de Boer, Gianni Pacella, Tobias van den Enk, Piermichele Kobauri, Giuseppe Portale, Christoph A Schalley*, Ben L Feringa*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

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Biological molecular machines enable chemical transformations, assembly, replication and motility, but most distinctively drive chemical systems out of-equilibrium to sustain life1,2. In such processes, nanometre-sized machines produce molecular energy carriers by driving endergonic equilibrium reactions. However, transforming the work performed by artificial nanomachines3-5 into chemical energy remains highly challenging. Here, we report a light-fuelled small-molecule ratchet capable of driving a coupled chemical equilibrium energetically uphill. By bridging two imine6-9 macrocycles with a molecular motor10,11, the machine forms crossings and consequently adopts several distinct topologies by either a thermal (temporary bond-dissociation) or photochemical (unidirectional rotation) pathway. While the former will relax the machine towards the global energetic minimum, the latter increases the number of crossings in the system above the equilibrium value. Our approach provides a blueprint for coupling continuous mechanical motion performed by a molecular machine with a chemical transformation to reach an out-of-equilibrium state.

Original languageEnglish
Pages (from-to)159-165
Number of pages7
JournalNature Nanotechnology
Early online date16-Dec-2021
Publication statusPublished - Feb-2022

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