Molecular-scale dissipative chemistry drives the formation of nanoscale assemblies and their macroscale transport.

IF 19.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nature chemistry Pub Date : 2024-11-08 DOI:10.1038/s41557-024-01665-z

Kai Liu, Alex W P Blokhuis, Sietse J Dijt, Juntian Wu, Shana Hamed, Armin Kiani, Bartosz M Matysiak, Sijbren Otto

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Abstract

Fuelled chemical systems have considerable functional potential that remains largely unexplored. Here we report an approach to transient amide bond formation and use it to harness chemical energy and convert it to mechanical motion by integrating dissipative self-assembly and the Marangoni effect in a source-sink system. Droplets are formed through dissipative self-assembly following the reaction of octylamine with 2,3-dimethylmaleic anhydride. The resulting amides are hydrolytically labile, making the droplets transient, which enables them to act as a source of octylamine. A sink for octylamine was created by placing a drop of oleic acid at the air-water interface. This source-sink system sets up a gradient in surface tension, which gives rise to a macroscopic Marangoni flow that can transport the droplets in solution with tunable speed. Carbodiimides can fuel this motion by converting diacid waste back to anhydride. This study shows how fuelling at the molecular level can, via assembly at the supramolecular level, lead to liquid flow at the macroscopic level.

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分子尺度的耗散化学推动了纳米尺度集合体的形成及其宏观传输。

燃料化学系统具有相当大的功能潜力，但在很大程度上尚未被开发。在这里，我们报告了一种瞬态酰胺键形成的方法，并通过在源-沉系统中整合耗散自组装和马兰戈尼效应，利用这种方法来利用化学能并将其转化为机械运动。辛胺与 2,3-二甲基马来酸酐反应后，通过耗散自组装形成液滴。生成的酰胺具有水解易变性，使液滴具有瞬时性，从而使液滴成为辛胺的来源。将一滴油酸滴在空气-水的界面上，就形成了辛胺的汇。这种源-汇系统会形成表面张力梯度，从而产生宏观的马兰戈尼流，以可调节的速度输送溶液中的液滴。碳二亚胺可以通过将二酸废料转化回酸酐来促进这种运动。这项研究展示了如何通过超分子水平的组装，在分子水平上提供动力，从而在宏观水平上产生液流。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nature chemistry 化学-化学综合

CiteScore

29.60

自引率

1.40%

发文量

226

审稿时长

1.7 months

期刊介绍： Nature Chemistry is a monthly journal that publishes groundbreaking and significant research in all areas of chemistry. It covers traditional subjects such as analytical, inorganic, organic, and physical chemistry, as well as a wide range of other topics including catalysis, computational and theoretical chemistry, and environmental chemistry. The journal also features interdisciplinary research at the interface of chemistry with biology, materials science, nanotechnology, and physics. Manuscripts detailing such multidisciplinary work are encouraged, as long as the central theme pertains to chemistry. Aside from primary research, Nature Chemistry publishes review articles, news and views, research highlights from other journals, commentaries, book reviews, correspondence, and analysis of the broader chemical landscape. It also addresses crucial issues related to education, funding, policy, intellectual property, and the societal impact of chemistry. Nature Chemistry is dedicated to ensuring the highest standards of original research through a fair and rigorous review process. It offers authors maximum visibility for their papers, access to a broad readership, exceptional copy editing and production standards, rapid publication, and independence from academic societies and other vested interests. Overall, Nature Chemistry aims to be the authoritative voice of the global chemical community.