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不同气体雾化的水微滴中二氧化碳无催化剂转化为小分子有机化合物

Catalyst-Free Transformation of Carbon Dioxide to Small Organic Compounds in Water Microdroplets Nebulized by Different Gases.

作者信息

Mehrgardi Masoud A, Mofidfar Mohammad, Li Jia, Chamberlayne Christian F, Lynch Stephen R, Zare Richard N

机构信息

Department of Chemistry, Stanford University, Stanford, California, 94305, USA.

Department of Chemistry, University of Isfahan, Isfahan, 81746, Iran.

出版信息

Adv Sci (Weinh). 2024 Oct;11(38):e2406785. doi: 10.1002/advs.202406785. Epub 2024 Aug 11.

DOI:10.1002/advs.202406785
PMID:39129358
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11481208/
Abstract

A straightforward nebulized spray system is designed to explore the hydrogenation of carbon dioxide (CO) within water microdroplets surrounded by different gases such as carbon dioxide, nitrogen, oxygen, and compressed air. The collected droplets are analyzed using water-suppressed nuclear magnetic resonance (NMR). Formate anion (HCOO), acetate anion (CHCOO), ethylene glycol (HOCHCHOH), and methane (CH) are detected when water is nebulized. This pattern persisted when the water is saturated with CO, indicating that CO in the nebulizing gas triggers the formation of these small organics. In a pure CO atmosphere, the formate anion concentration is determined to be ≈70 µm, referenced to dimethyl sulfoxide, which has been introduced as an internal standard in the collected water droplets. This study highlights the power of water microdroplets to initiate unexpected chemistry for the transformation of CO to small organic compounds.

摘要

设计了一种简单的雾化喷雾系统,用于探索在由二氧化碳、氮气、氧气和压缩空气等不同气体包围的水微滴中二氧化碳(CO)的氢化反应。使用水抑制核磁共振(NMR)对收集到的液滴进行分析。雾化水时检测到甲酸根阴离子(HCOO)、乙酸根阴离子(CHCOO)、乙二醇(HOCHCHOH)和甲烷(CH)。当水用CO饱和时,这种模式仍然存在,这表明雾化气体中的CO触发了这些小有机物的形成。在纯CO气氛中,以二甲基亚砜为参比,确定收集到的水滴中引入的内标物,甲酸根阴离子浓度约为70 µm。这项研究突出了水微滴引发将CO转化为小有机化合物的意外化学反应的能力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b42f/11481208/eb9dfc058145/ADVS-11-2406785-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b42f/11481208/5b6a0bf12aee/ADVS-11-2406785-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b42f/11481208/d2564cd50cf6/ADVS-11-2406785-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b42f/11481208/636e87d69177/ADVS-11-2406785-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b42f/11481208/eb9dfc058145/ADVS-11-2406785-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b42f/11481208/5b6a0bf12aee/ADVS-11-2406785-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b42f/11481208/d2564cd50cf6/ADVS-11-2406785-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b42f/11481208/636e87d69177/ADVS-11-2406785-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b42f/11481208/eb9dfc058145/ADVS-11-2406785-g005.jpg

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本文引用的文献

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Charged Microdroplets as Microelectrochemical Cells for CO Reduction and C-C Coupling.用于CO还原和C-C偶联的带电微滴作为微电化学电池
J Am Chem Soc. 2024 Jan 24;146(3):2227-2236. doi: 10.1021/jacs.3c12586. Epub 2024 Jan 15.
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Significant Acceleration of Photocatalytic CO Reduction at the Gas-Liquid Interface of Microdroplets.
在微液滴的气-液界面处显著加速光催化 CO 还原。
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Probing dissolved CO(aq) in aqueous solutions for CO electroreduction and storage.探测水溶液中溶解的CO(aq)用于CO电还原和储存。
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Can electric fields drive chemistry for an aqueous microdroplet?电场能驱动水溶液微滴中的化学反应吗?
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Aqueous microdroplets containing only ketones or aldehydes undergo Dakin and Baeyer-Villiger reactions.仅含有酮或醛的水性微滴会发生达金反应和拜耳-维利格反应。
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Electrochemical CO reduction to high-concentration pure formic acid solutions in an all-solid-state reactor.在全固态反应器中将电化学CO还原为高浓度纯甲酸溶液。
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Simple model for the electric field and spatial distribution of ions in a microdroplet.微滴中离子电场和空间分布的简单模型。
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