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化学燃料驱动的多任务处理:由五个不同组分耗散形成假轮烷转子

Multitasking with Chemical Fuel: Dissipative Formation of a Pseudorotaxane Rotor from Five Distinct Components.

作者信息

Ghosh Amit, Paul Indrajit, Schmittel Michael

机构信息

Center of Micro- and Nanochemistry and Engineering, Organische Chemie I, Universität Siegen, Adolf-Reichwein-Strasse 2, D-57068 Siegen, Germany.

出版信息

J Am Chem Soc. 2021 Apr 14;143(14):5319-5323. doi: 10.1021/jacs.1c01948. Epub 2021 Mar 31.

Abstract

A 3-fold completive self-sorted library of dynamic motifs was integrated into the design of the pseudorotaxane-based rotor [Zn(·H)()()] operating at = 15.4 kHz. The rotational motion in the five-component device is based on association/dissociation of the pyridyl head of the pseudorotaxane rotator arm between two zinc(II) porphyrin stations. Addition of TFA or 2-cyano-2-phenylpropanoic acid as a chemical fuel to a zinc release system and the loose rotor components - enabled the liberated zinc(II) ions and protons to act in unison, setting up the rotor through the formation of a heteroleptic zinc complex and a pseudorotaxane linkage. With chemical fuel, the dissipative system was reproducibly pulsed three times without a problem. Due to the double role of the fuel acid, two kinetically distinct processes played a role in both the out-of-equilibrium assembly and disassembly of the rotor, highlighting the complex issues in multitasking of chemical fuels.

摘要

一个具有3倍竞争力的动态基序自分类库被整合到基于准轮烷的转子[Zn(·H)()()]的设计中,该转子在15.4 kHz下运行。五组分装置中的旋转运动基于准轮烷旋转臂的吡啶基头部在两个锌(II)卟啉位点之间的缔合/解离。向锌释放系统和松散的转子组件中添加三氟乙酸或2-氰基-2-苯基丙酸作为化学燃料,使释放出的锌(II)离子和质子协同作用,通过形成异核锌配合物和准轮烷键来启动转子。使用化学燃料时,耗散系统可重复脉冲三次而无问题。由于燃料酸的双重作用,两个动力学上不同的过程在转子的非平衡组装和解组装中都发挥了作用,突出了化学燃料多任务处理中的复杂问题。

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