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ATP驱动的自组装在时域内调节化学反应性
ATP-fuelled self-assembly to regulate chemical reactivity in the time domain

Chemical Science(中文翻译) ( IF 9.556 ) Pub Date : 2019-12-18 , DOI: 10.1039/c9sc05188k
Leonard JanPrins; Maria ACardona

作者利用一种小生物分子ATP实现了由小自组装分子组成的合成体系中化学反应性的时间控制。该方法依赖于ATP模板化基于两亲物的组装体的形成的能力。碱性磷酸酶的存在会导致ATP浓度随时间逐渐降低,从而导致组装体自发解离。组装体疏水域中非极性反应物的吸收可提高反应速率。结果表明,ATP触发的自组装会导致体系中同时发生的两个腙键形成反应中的一个选择性上调。这导致产物比率的反转,但是,这实际上是暂时的,因为一旦ATP被酶消耗,上调的反应就会自发地恢复到其基本的低反应速率。总体而言,结果表明,在耗散条件下化学驱动的自组装可获得复杂化学体系的时间控制。
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Here, we exploit a small biomolecule – ATP – to gain temporal control over chemical reactivity in a synthetic system composed of small self-assembling molecules and reactants. The approach relies on the capacity of ATP to template the formation of amphiphile-based assemblies. The presence of the enzyme alkaline phosphatase causes a gradual decrease in the ATP-concentration in time and, consequently, a spontaneous dissociation of the assemblies. The uptake of apolar reactants in the hydrophobic domain of the assemblies leads to an enhancement of the reaction rate. It is shown that ATP-triggered self-assembly causes the selective upregulation of one out of two hydrazone-bond formation reactions that take place concurrently in the system. This leads to an inversion in the product ratio, which, however, is transient in nature because the upregulated reaction spontaneously reverts to its basal low reaction rate once the ATP has been consumed by the enzyme. Overall, the results demonstrate the potential of chemically-fuelled self-assembly under dissipative conditions to gain temporal control over reactivity in complex chemical systems.
更新日期:2019-12-19

 

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