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等离子体中CH的部分氧化：添加氧化剂和催化剂的影响。

Partial Oxidation of CH in Plasma: The Effects of Oxidant and Catalyst Addition.

作者信息

Golubev Oleg V, Maximov Anton L

机构信息

A.V. Topchiev Institute of Petrochemical Synthesis, Russian Academy of Sciences (TIPS RAS), Moscow 119991, Russia.

出版信息

Molecules. 2025 Apr 28;30(9):1958. doi: 10.3390/molecules30091958.

DOI:10.3390/molecules30091958
PMID:40363765
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12074086/
Abstract

The partial oxidation of methane in cold atmospheric plasma represents an innovative and promising approach to energy conversion and sustainable chemical processes for obtaining various chemicals and fuels. In present work, dielectric barrier discharge plasma is applied to the partial oxidation of CH combined with Cu-containing catalysts. The catalysts with different porous and acidic properties were obtained, characterized by physico-chemical methods and used in plasma-catalytic reaction. The influence of the oxidizing agent (oxygen vs. air) on the products' selectivity and yield was studied. It was found that using air as an oxidizer was beneficial in terms of CH conversion and gaseous products yield, as N aided in denser microdischarge formation. Using pure O for methane partial oxidation resulted in enhanced oxygenate (mainly CHOH) generation. Furthermore, the Cu-containing catalysts enhanced methanol yield compared to the plasma-only process, as well as the energy efficiency of the process.

摘要

冷大气等离子体中甲烷的部分氧化是一种创新且有前景的能量转换和可持续化学过程的方法，可用于获得各种化学品和燃料。在当前工作中，将介质阻挡放电等离子体应用于CH与含铜催化剂结合的部分氧化过程。制备了具有不同多孔性和酸性的催化剂，通过物理化学方法对其进行表征，并用于等离子体催化反应。研究了氧化剂（氧气与空气）对产物选择性和产率的影响。结果发现，使用空气作为氧化剂有利于CH的转化和气态产物的产率，因为N有助于形成更密集的微放电。使用纯O进行甲烷部分氧化可提高含氧化合物（主要是CHOH）的生成量。此外，与仅等离子体过程相比，含铜催化剂提高了甲醇产率以及该过程的能量效率。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/18d49fe866cc/molecules-30-01958-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/16886db7814b/molecules-30-01958-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/4733bbb56d48/molecules-30-01958-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/2d598c4f4914/molecules-30-01958-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/8508a4f78a0d/molecules-30-01958-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/ce2fc54161e7/molecules-30-01958-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/86520fafdca2/molecules-30-01958-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/18d49fe866cc/molecules-30-01958-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/16886db7814b/molecules-30-01958-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/4733bbb56d48/molecules-30-01958-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/2d598c4f4914/molecules-30-01958-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/8508a4f78a0d/molecules-30-01958-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/ce2fc54161e7/molecules-30-01958-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/86520fafdca2/molecules-30-01958-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c63f/12074086/18d49fe866cc/molecules-30-01958-g007.jpg

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本文引用的文献

1
Direct Methane to Methanol Conversion: An Overview of Non-Syn Gas Catalytic Strategies.直接甲烷制甲醇转化：非合成气催化策略概述
Chem Rec. 2025 Jan 16;25(2):e202400186. doi: 10.1002/tcr.202400186.
2
Methane-to-chemicals: a pathway to decarbonization.甲烷转化为化学品：一条脱碳途径。
Natl Sci Rev. 2023 Apr 25;10(9):nwad116. doi: 10.1093/nsr/nwad116. eCollection 2023 Sep.
3
The Direct Catalytic Oxidation of Methane to Methanol-A Critical Assessment.甲烷直接氧化制甲醇的研究进展。
Angew Chem Int Ed Engl. 2017 Dec 22;56(52):16464-16483. doi: 10.1002/anie.201702550. Epub 2017 Nov 22.
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Methane as raw material in synthetic chemistry: the final frontier.甲烷作为合成化学中的原料：最后的前沿。
Chem Soc Rev. 2013 Dec 7;42(23):8809-20. doi: 10.1039/c3cs60120j. Epub 2013 Aug 19.
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Platinum catalysts for the high-yield oxidation of methane to a methanol derivative.用于将甲烷高产率氧化为甲醇衍生物的铂催化剂。
Science. 1998 Apr 24;280(5363):560-4. doi: 10.1126/science.280.5363.560.