Wang Peng-Lai, Borsley Stefan, Power Martin J, Cavasso Alessandro, Giuseppone Nicolas, Leigh David A
Department of Chemistry, University of Manchester, Manchester, UK.
School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, China.
Nature. 2025 Jan;637(8046):594-600. doi: 10.1038/s41586-024-08288-x. Epub 2025 Jan 15.
Cells display a range of mechanical activities generated by motor proteins powered through catalysis. 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 catalyst. Here we demonstrate the molecular-level transduction of chemical energy to mechanical force 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-driven molecular motors. Continuous 360° 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 transduction, informs both the debate surrounding the mechanism of force generation by biological motors and the design principles for artificial molecular nanotechnology.
细胞展现出一系列由通过催化提供动力的马达蛋白所产生的机械活动。这就引出了一个基本问题:化学反应的加速如何能使该反应释放的能量被分子催化剂转导(进而完成功)。在此,我们展示了化学能到机械能的分子水平转导,其形式为通过人工催化驱动的分子马达的定向旋转来驱动交联聚合物凝胶进行动力收缩和动力再膨胀。嵌入凝胶聚合物框架中的催化驱动马达分子的转子围绕定子连续进行360°旋转,使交联网络的聚合物链相互缠绕扭曲。这逐渐增加了缠绕并收紧了缠结,导致凝胶宏观收缩至其原始体积的约70%。随后添加相反对映体的供能系统,驱动马达分子反向旋转,解开缠结并使凝胶再膨胀。在新方向上持续对链进行动力扭曲会导致凝胶再次收缩。除了驱动作用外,凝胶中马达分子的旋转还会产生其他化学和物理结果,包括杨氏模量和储能模量的变化——后者与马达旋转导致的链交叉增加成正比。合成有机催化剂对抗负载做功的实验演示及其能量转导机制,既为围绕生物马达力产生机制的争论提供了信息,也为人工分子纳米技术的设计原则提供了信息。