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钯促进由低级胺原料生产高级胺。

Palladium Promoted Production of Higher Amines from a Lower Amine Feedstock.

作者信息

Hao Yufen, Cárdenas-Lizana Fernando, Keane Mark A

机构信息

Chemical Engineering, School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh, EH14 4AS Scotland, UK.

出版信息

Catal Letters. 2017;147(4):803-810. doi: 10.1007/s10562-016-1902-7. Epub 2017 Feb 14.

DOI:10.1007/s10562-016-1902-7
PMID:32226263
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7089641/
Abstract

ABSTRACT

The catalytic (Pd/AlO and Pd/C; mean Pd size 2.5-3.0 nm from (S)TEM analysis) synthesis of di-butylamine (DBA) and tri-butylamine (TBA) from mono-butylamine (MBA) and DBA, respectively, in continuous gas phase operation is demonstrated. Exclusive production of DBA (from MBA) has been established over both catalysts where 453 ≤  ≤ 523 K (∆E = 79 kJ mol). Greater activity for Pd/C is associated with higher levels of surface acidity (from NH chemisorption/TPD) and spillover hydrogen (from H TPD). Reaction of DBA over both catalysts when configured in series delivered full selectivity to TBA. Our results establish a novel clean alternative route for the continuous production of higher (secondary and tertiary) amines.

摘要

摘要

本文展示了在连续气相操作中，分别以单丁胺（MBA）和二丁胺（DBA）为原料，通过催化作用（Pd/AlO和Pd/C；经（S）TEM分析，平均钯粒径为2.5 - 3.0纳米）合成二丁胺（DBA）和三丁胺（TBA）的过程。在两种催化剂上均已实现从MBA独家生产DBA，反应温度为453 ≤ ≤ 523 K（∆E = 79 kJ mol）。Pd/C具有更高的活性，这与更高水平的表面酸度（通过NH化学吸附/TPD测定）和溢流氢（通过H TPD测定）有关。当两种催化剂串联配置时，DBA在两种催化剂上的反应对TBA具有完全选择性。我们的研究结果为连续生产高级（仲胺和叔胺）胺建立了一种新型的清洁替代路线。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/53407d8f3538/10562_2016_1902_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/c40e05ba10e1/10562_2016_1902_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/204fe8b1a0b8/10562_2016_1902_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/552513abf09f/10562_2016_1902_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/42ece0a67883/10562_2016_1902_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/5a5e4d914634/10562_2016_1902_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/53407d8f3538/10562_2016_1902_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/c40e05ba10e1/10562_2016_1902_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/204fe8b1a0b8/10562_2016_1902_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/552513abf09f/10562_2016_1902_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/42ece0a67883/10562_2016_1902_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/5a5e4d914634/10562_2016_1902_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/54fa/7089641/53407d8f3538/10562_2016_1902_Fig6_HTML.jpg

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本文引用的文献

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Highly efficient heterogeneous gold-catalyzed direct synthesis of tertiary and secondary amines from alcohols and urea.高效的非均相金催化醇和尿素直接合成叔胺和仲胺。
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