重新利用催化循环进行瞬态自组装。
Repurposing a Catalytic Cycle for Transient Self-Assembly.
作者信息
Amano Shuntaro, Hermans Thomas M
机构信息
University of Strasbourg, CNRS, Strasbourg 67083, France.
IMDEA Nanociencia, Madrid 28049, Spain.
出版信息
J Am Chem Soc. 2024 Aug 21;146(33):23289-23296. doi: 10.1021/jacs.4c05871. Epub 2024 Aug 11.
Life operates out of equilibrium to enable various sophisticated behaviors. Synthetic chemists have strived to mimic biological nonequilibrium systems in such fields as autonomous molecular machines and dissipative self-assembly. Central to these efforts has been the development of new chemical reaction cycles, which drive systems out of equilibrium by conversion of chemical fuel into waste species. However, the construction of reaction cycles has been challenging due to the difficulty of finding compatible reactions that constitute a cycle. Here, we realize an alternative approach by repurposing a known catalytic cycle as a chemical reaction cycle for driving dissipative self-assembly. This approach can overcome the compatibility problem because all steps involved in a catalytic cycle are already known to proceed concurrently under the same conditions. Our repurposing approach is applicable to diverse combinations of catalytic cycles and systems to drive out of equilibrium, which will substantially broaden the scope of out-of-equilibrium systems.
生命在非平衡状态下运行,以实现各种复杂行为。合成化学家一直致力于在自主分子机器和耗散性自组装等领域模拟生物非平衡系统。这些努力的核心是开发新的化学反应循环,通过将化学燃料转化为废物来驱使系统偏离平衡状态。然而,由于难以找到构成一个循环的兼容反应,反应循环的构建一直具有挑战性。在这里,我们通过将一个已知的催化循环重新用作驱动耗散性自组装的化学反应循环,实现了一种替代方法。这种方法可以克服兼容性问题,因为已知催化循环中涉及的所有步骤在相同条件下同时进行。我们的重新利用方法适用于催化循环和系统的各种组合,以驱使它们偏离平衡状态,这将大大拓宽非平衡系统的范围。