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Induction of motion in a synthetic molecular machine: Effect of tuning the driving force

机译：合成分子机器中的运动感应：调整驱动力的效果

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Rotaxane molecular shuttles were studied in which a tetralactam macrocyclic ring moves between a succinamide station and a second station in which the structure is varied. Station2 in all cases is an aromatic imide, which is a poor hydrogen-bond acceptor in the neutral form, but a strong one when reduced with one or two electrons. When the charge density on the hydrogen-bond-accepting carbonyl groups in station2 is reduced by changing a naphthalimide into a naphthalene diimide radical anion, the shuttling rate changes only slightly. When station2 is a pyromellitimide radical anion, however, the shuttling rate is significantly reduced. This implies that the shuttling rate is not only determined by the initial unbinding of the ring from the first station, as previously supposed. An alternative reaction mechanism is proposed in which the ring binds to both stations in the transition state. Shuttling via harpooning: Comparison of the shuttling kinetics in a series of imide-based rotaxanes suggest that the mechanism involves a transition state in which the moving ring is hydrogen-bonded to both stations (see figure).
机译：研究了轮烷的分子穿梭，其中四内酰胺大环在琥珀酰胺站和结构发生变化的第二站之间移动。在所有情况下，Station2都是芳族酰亚胺，它是中性形式的弱氢键受体，但在被一个或两个电子还原时却是一个强酰亚胺。当通过将萘二甲酰亚胺转变为萘二甲酰亚胺自由基阴离子而降低工位2中的氢键接受羰基上的电荷密度时，穿梭速率仅稍有变化。但是，当station2是均苯四甲酰亚胺基自由基阴离子时，穿梭速率会大大降低。这意味着，穿梭速率不仅取决于环与第一站点的初始解除绑定，如先前所假定的那样。提出了另一种反应机理，其中环在过渡态与两个位置结合。通过鱼叉进行穿梭：在一系列基于酰亚胺的轮烷中的穿梭动力学比较表明，该机理涉及过渡态，其中动环氢键合到两个位点（见图）。

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