Transducing chemical energy through catalysis by an artificial molecular motor

• 成果类型: Article
• 署名作者: Wang, Peng-Lai; Borsley, Stefan; Power, Martin J.; Cavasso, Alessandro; Giuseppone, Nicolas; Leigh, David A.
• 署名单位: University of Manchester; East China Normal University; Universites de Strasbourg Etablissements Associes; Universite de Strasbourg; Institut Universitaire de France
• 刊物名称: Nature
• ISSN/ISSBN: 0028-2105
• DOI: 10.1038/s41586-024-08288-x
• 发表日期: 2025-01-16
• 关键词: driven; rotation; rotary

摘要

Cells display a range of mechanical activities generated by motor proteins powered through catalysis1. This raises the fundamental question of how the acceleration of a chemical reaction can enable the energy released from that reaction to be transduced (and, consequently, work to be done) by a molecular catalyst2, 3, 4, 5, 6-7. Here we demonstrate the molecular-level transduction of chemical energy to mechanical force8 in the form of the powered contraction and powered re-expansion of a cross-linked polymer gel driven by the directional rotation of artificial catalysis-driven9 molecular motors. Continuous 360 degrees rotation of the rotor about the stator of the catalysis-driven motor-molecules incorporated in the polymeric framework of the gel twists the polymer chains of the cross-linked network around one another. This progressively increases writhe and tightens entanglements, causing a macroscopic contraction of the gel to approximately 70% of its original volume. The subsequent addition of the opposite enantiomer fuelling system powers the rotation of the motor-molecules in the reverse direction, unwinding the entanglements and causing the gel to re-expand. Continued powered twisting of the strands in the new direction causes the gel to re-contract. In addition to actuation, motor-molecule rotation in the gel produces other chemical and physical outcomes, including changes in the Young modulus and storage modulus-the latter is proportional to the increase in strand crossings resulting from motor rotation. The experimental demonstration of work against a load by a synthetic organocatalyst, and its mechanism of energy transduction6, informs both the debate3,5,7 surrounding the mechanism of force generation by biological motors and the design principles6,10, 11, 12, 13-14 for artificial molecular nanotechnology.