A gold-nanoparticle stoppered [2]rotaxane†,Nanoscale

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A gold-nanoparticle stoppered [2]rotaxane†
Nanoscale ( IF 5.8 ) Pub Date : 2018-05-03 00:00:00 , DOI: 10.1039/c8nr01622d
Anne Ulfkjær _{1,

2,

3,

4} , Frederik W. Nielsen _{1,

2,

3,

4} , Hana Al-Kerdi _{1,

2,

3,

4} , Tamara Ruβ _{1,

2,

3,

4} , Zaki K. Nielsen _{1,

2,

3,

4} , Jens Ulstrup _{1,

4,

5,

6} , Lanlan Sun _{7,

8,

9,

10} , Kasper Moth-Poulsen _{7,

8,

9,

10} , Jingdong Zhang _{1,

4,

5,

6} , Michael Pittelkow _{1,

2,

3,

4}

Affiliation

The construction of molecular machines has captured the imagination of scientists for decades. Despite significant progress in the synthesis and studies of the properties of small-molecule components (smaller than 2–5 kilo Dalton), challenges regarding the incorporation of molecular components into real devices are still eminent. Nano-sized molecular machines operate the complex biological machinery of life, and the idea of mimicking the amazing functions using artificial nano-structures is intriguing. Both in small-molecule molecular machine components and in many naturally occurring molecular machines, mechanically interlocked molecules and structures are key functional components. In this work, we describe our initial efforts to interface mechanically-interlocked molecules and gold-nanoparticles (AuNPs); the molecular wire connecting the AuNPs is covered in an insulating rotaxane-layer, thus mimicking the macroscopic design of a copper wire. Taking advantage of recent progress in the preparation of supramolecular complexes of the cucurbit[7]uril (CB[7]) macrocycle, we have prepared a bis-thiol functionalised pseudo-rotaxane that enables us to prepare a AuNP-stoppered [2]rotaxane in water. The pseudo-rotaxane is held together extremely tightly (K_a > 10¹³ M⁻¹), K_a being the association constant. We have studied the solution and gas phase guest–host chemistry using NMR spectroscopy, mass spectroscopy, and electrochemistry. The bis-thiol functionalised pseudo-rotaxane holds further a ferrocene unit in the centre of the rotaxane; this ferrocene unit enables us to address the system in detail with and without CB[7] and AuNPs using electrochemical methods.

中文翻译：

纳米金颗粒塞住的[2]轮烷†

数十年来，分子机器的构造吸引了科学家的想象力。尽管在合成和研究小分子组分（小于2至5千道尔顿）的性能方面取得了显着进展，但仍然存在着将分子组分结合到实际装置中的挑战。纳米分子机器操作着生命的复杂生物机器，并且使用人工纳米结构模仿惊人功能的想法引起了人们的兴趣。在小分子分子机器组件和许多自然发生的分子机器中，机械互锁的分子和结构都是关键的功能组件。在这项工作中，我们描述了我们为使机械互锁的分子与金纳米粒子（AuNPs）接触而做出的初步努力。连接AuNPs的分子线被绝缘的轮烷层覆盖，从而模仿了铜线的宏观设计。利用最近制备葫芦[7] uril（CB [7]）的超分子复合物的进展，我们制备了一种双硫醇官能化的假轮烷，可以制备以AuNP封端的[2]轮烷。在水里。假轮烷非常紧密地结合在一起（K _a＞ 10 ¹³ M ^-1），K _a为缔合常数。我们已经使用NMR光谱，质谱和电化学方法研究了溶液和气相客体-主体化学。双硫醇官能化的假轮烷在轮烷的中心还具有一个二茂铁单元。该二茂铁单元使我们能够使用电化学方法在有或没有CB [7]和AuNPs的情况下详细处理该系统。

更新日期：2018-05-03

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