Aix Marseille Univ, CNRS, ICR, Marseille, France.
State Key Laboratory of Quality Research in Chinese Medicine, Institute of Chinese Medical Sciences, University of Macau, Avenida da Universidade, Taipa, Macau, China.
Angew Chem Int Ed Engl. 2021 Mar 15;60(12):6617-6623. doi: 10.1002/anie.202014399. Epub 2021 Feb 10.
Molecular machines are ubiquitous in nature and function away from equilibrium by consuming fuels to produce appropriate work. Chemists have recently excelled at mimicking the fantastic job performed by natural molecular machines with synthetic systems soluble in organic solvents. In efforts toward analogous systems working in water, we show that guest molecules can be exchanged in the synthetic macrocycle cucurbit[7]uril by involving kinetic traps, and in such a way as modulating energy wells and kinetic barriers using pH, light, and redox stimuli. Ditolyl-viologen can also be exchanged using the best kinetic trap and interfaced with alginate, thus affording pH-responsive blue, fluorescent hydrogels. With tunable rate and binding constants toward relevant guests, cucurbiturils may become excellent ring molecules for the construction of advanced molecular machines working in water.
分子机器在自然界中无处不在，它们通过消耗燃料来产生适当的功，从而在远离平衡的状态下发挥作用。化学家们最近在模拟天然分子机器的奇妙工作方面取得了卓越的成就，他们使用的是在有机溶剂中可溶的合成系统。在努力构建类似的在水中工作的系统时，我们表明，通过引入动力学陷阱，客体分子可以在合成大环瓜环[7]脲中进行交换，并且可以通过 pH 值、光和氧化还原刺激来调节能量势阱和动力学障碍。二芐基-紫精也可以使用最佳的动力学陷阱进行交换，并与藻酸盐接口，从而提供 pH 响应的蓝色荧光水凝胶。具有针对相关客体的可调速率和结合常数，瓜环可能成为构建在水中工作的高级分子机器的优秀环分子。
