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未活化微滴的微滴化学

Microdroplet Chemistry with Unactivated Droplets.

作者信息

Chen Huan, Li Xiaoxu, Li Bowen, Chen Yeye, Ouyang Haoran, Li Youcun, Zhang Xinxing

机构信息

College of Chemistry, State Key Laboratory of Advanced Chemical Power Sources, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Renewable Energy Conversion and Storage Centre, Tianjin Key Laboratory of Biosensing and Molecular Recognition, Frontiers Science Centre for New Organic Matter, Nankai University, Tianjin, 300071, China.

出版信息

J Am Chem Soc. 2025 Apr 2;147(13):11399-11406. doi: 10.1021/jacs.5c01072. Epub 2025 Mar 22.

DOI:10.1021/jacs.5c01072
PMID:40119802
Abstract

Microdroplet chemistry has attracted much attention owing to its ability to accelerate otherwise slow reactions and to trigger thermodynamically forbidden reactions. The cause of this unique behavior is the intrinsic properties of the droplets, such as the spontaneously generated electric field on the droplet surface. However, some have argued that the droplet generation methods provided energy to the reactions, and the different interfaces that the droplets contact also played important roles; therefore, it is the droplet activation or the environment, not the intrinsic properties, that is responsible for the observed chemistry. In this study, we used adiabatic expansion and dry ice in water to generate homogeneous, contactless, supercooled, and unactivated microdroplets. A large variety of reactions were successfully tested. We opine that it is the intrinsic properties, and not droplet activation, that are responsible for microdroplet chemistry.

摘要

微滴化学因其能够加速原本缓慢的反应并引发热力学上禁止的反应而备受关注。这种独特行为的原因是液滴的固有特性,例如液滴表面自发产生的电场。然而,一些人认为液滴生成方法为反应提供了能量,并且液滴接触的不同界面也起到了重要作用;因此,是液滴活化或环境而非固有特性导致了所观察到的化学反应。在本研究中,我们使用绝热膨胀和水中干冰来生成均匀、无接触、过冷且未活化的微滴。成功测试了各种各样的反应。我们认为是固有特性而非液滴活化导致了微滴化学。

相似文献

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Microdroplet Chemistry with Unactivated Droplets.未活化微滴的微滴化学
J Am Chem Soc. 2025 Apr 2;147(13):11399-11406. doi: 10.1021/jacs.5c01072. Epub 2025 Mar 22.
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Microdroplet-Mediated Radical Polymerization.微滴介导的自由基聚合
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引用本文的文献

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Mechanisms of ionization and of chemical reactions in charged microdroplets.带电微滴中的电离机制和化学反应机制。
Chem Sci. 2025 Sep 4. doi: 10.1039/d5sc04781a.
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Electric field-driven interfacial reduction of metal ions in microdroplets: gold, silver, and nickel.微滴中金属离子的电场驱动界面还原:金、银和镍。
Chem Sci. 2025 Jul 29. doi: 10.1039/d5sc04995d.
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Synthesis of benzoquinone compounds by a microdroplet-accelerated retro-Diels-Alder reaction.通过微滴加速逆狄尔斯-阿尔德反应合成苯醌化合物。
Chem Sci. 2025 Jul 3. doi: 10.1039/d5sc03761a.
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An Alternative Explanation for Ions Put Forth as Evidence for Abundant Hydroxyl Radicals Formed Due to the Intrinsic Electric Field at the Surface of Water Droplets.关于作为水滴表面固有电场形成大量羟基自由基证据而提出的离子的另一种解释。
Anal Chem. 2025 Aug 19;97(32):17687-17695. doi: 10.1021/acs.analchem.5c02973. Epub 2025 Jun 26.