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在近临界乙腈条件下,甲烷在氮化硼上部分氧化生成甲醇。

Partial oxidation of methane to methanol on boron nitride at near critical acetonitrile.

作者信息

Kapuge Tharindu Kankanam, Moharreri Ehsan, Perera Inosh, Eddy Nicholas, Kriz David, Nisly Nathaniel, Shuster Seth, Nandi Partha, Suib Steven L

机构信息

Department of Chemistry, University of Connecticut, Storrs, CT, 06269, USA.

Institute of Material Science, University of Connecticut, Storrs, CT, 06269, USA.

出版信息

Sci Rep. 2022 May 20;12(1):8577. doi: 10.1038/s41598-022-12639-x.

DOI:10.1038/s41598-022-12639-x
PMID:35595791
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9122901/
Abstract

Direct catalytic conversion of methane to methanol with O has been a fundamental challenge in unlocking abundant natural gas supplies. Metal-free methane conversion with 17% methanol yield based on the limiting reagent O at 275 °C was achieved with near supercritical acetonitrile in the presence of boron nitride. Reaction temperature, catalyst loading, dwell time, methane-oxygen molar ratio, and solvent-oxygen molar ratios were identified as critical factors controlling methane activation and the methanol yield. Extension of the study to ethane (C2) showed moderate yields of methanol (3.6%) and ethanol (4.5%).

摘要

将甲烷与氧气直接催化转化为甲醇一直是释放丰富天然气供应的一项根本性挑战。在氮化硼存在的情况下,使用近超临界乙腈在275°C实现了基于限量试剂氧气的无金属甲烷转化,甲醇产率为17%。反应温度、催化剂负载量、停留时间、甲烷-氧气摩尔比和溶剂-氧气摩尔比被确定为控制甲烷活化和甲醇产率的关键因素。将该研究扩展到乙烷(C₂)显示甲醇(3.6%)和乙醇(4.5%)的产率适中。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/008ca6d61ef8/41598_2022_12639_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/b30728b739f8/41598_2022_12639_Fig1_HTML.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/0b54df0030f7/41598_2022_12639_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/aef68c8441b9/41598_2022_12639_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/641b151156f1/41598_2022_12639_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/7e1d174d02df/41598_2022_12639_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/36660cc0d2a9/41598_2022_12639_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/008ca6d61ef8/41598_2022_12639_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/b30728b739f8/41598_2022_12639_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/2fc4f50128a9/41598_2022_12639_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/0b54df0030f7/41598_2022_12639_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/aef68c8441b9/41598_2022_12639_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/641b151156f1/41598_2022_12639_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/7e1d174d02df/41598_2022_12639_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/36660cc0d2a9/41598_2022_12639_Fig7_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/1758/9122901/008ca6d61ef8/41598_2022_12639_Fig8_HTML.jpg

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Direct conversion of methane to formaldehyde and CO on BO catalysts.
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