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研究胺类在集成式二氧化碳捕集与利用中的质子穿梭和电化学机制。

Investigating proton shuttling and electrochemical mechanisms of amines in integrated CO capture and utilization.

作者信息

Bruggeman D F, Rothenberg G, Garcia A C

机构信息

Van't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, Amsterdam, The Netherlands.

出版信息

Nat Commun. 2024 Oct 24;15(1):9207. doi: 10.1038/s41467-024-53543-4.

DOI:10.1038/s41467-024-53543-4
PMID:39448574
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11502734/
Abstract

Carbon capture and utilization (CCU) technologies present a promising solution for converting CO emissions into valuable products. Here we show how amines, such as monoethanolamine (MEA) and 2-amino-2-methyl-1-propanol (AMP), influence the electrochemical CO reduction process in an integrated CCU system. Using in situ spectroscopic techniques, we identify the key roles of carbamate bond strength, proton shuttling, and amine structure in dictating reaction pathways on copper (Cu) and lead (Pb) electrodes. Our findings demonstrate that on Cu electrodes, surface blockage by ammonium species impedes CO₂ reduction, whereas on Pb electrodes, proton shuttling enhances the production of hydrocarbon products. This study provides additional insights into optimizing CCU systems by tailoring the choice of amines and electrode materials, advancing the selective conversion of CO₂ into valuable chemicals.

摘要

碳捕获与利用(CCU)技术为将二氧化碳排放转化为有价值的产品提供了一个很有前景的解决方案。在此,我们展示了胺类物质,如单乙醇胺(MEA)和2-氨基-2-甲基-1-丙醇(AMP),如何在集成CCU系统中影响电化学二氧化碳还原过程。通过使用原位光谱技术,我们确定了氨基甲酸盐键强度、质子穿梭和胺结构在决定铜(Cu)和铅(Pb)电极上的反应途径中的关键作用。我们的研究结果表明,在铜电极上,铵类物质造成的表面堵塞会阻碍二氧化碳还原,而在铅电极上,质子穿梭会提高烃类产品的产量。这项研究通过定制胺类和电极材料的选择,为优化CCU系统提供了更多见解,推动了将二氧化碳选择性转化为有价值化学品的进程。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/5a618bb6f778/41467_2024_53543_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/c52a01d272e6/41467_2024_53543_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/6a542032cdab/41467_2024_53543_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/97c420f0c76c/41467_2024_53543_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/9e82373a7e28/41467_2024_53543_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/5a618bb6f778/41467_2024_53543_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/c52a01d272e6/41467_2024_53543_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/6a542032cdab/41467_2024_53543_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/97c420f0c76c/41467_2024_53543_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/9e82373a7e28/41467_2024_53543_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/038f/11502734/5a618bb6f778/41467_2024_53543_Fig5_HTML.jpg

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ACS Cent Sci. 2023 Sep 26;9(10):1905-1912. doi: 10.1021/acscentsci.3c00826. eCollection 2023 Oct 25.
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Tailoring Electrochemical CO Reduction on Copper by Reactive Ionic Liquid and Native Hydrogen Bond Donors.
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Angew Chem Int Ed Engl. 2024 Jan 2;63(1):e202312163. doi: 10.1002/anie.202312163. Epub 2023 Nov 6.
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Solvent Effect on Electrochemical CO Reduction Reaction on Nanostructured Copper Electrodes.溶剂对纳米结构铜电极上电化学CO还原反应的影响
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Infrared action spectroscopy of the deprotonated formic acid trimer, trapped in helium nanodroplets.捕获于氦纳米液滴中的去质子化甲酸三聚体的红外作用光谱。
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