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固载钌和富胺催化体系中 CO 和氢气的预捕获及甲醇加氢反应。

Precapture of CO and Hydrogenation into Methanol on Heterogenized Ruthenium and Amine-Rich Catalytic Systems.

机构信息

Department of Materials and Environmental Chemistry, Stockholm University, 10691, Stockholm, Sweden.

Current address: Cambrex Karlskoga AB, 691 33, Karlskoga, Sweden.

出版信息

ChemistryOpen. 2023 Jun;12(6):e202300060. doi: 10.1002/open.202300060.

DOI:10.1002/open.202300060
PMID:37259697
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10233216/
Abstract

A heterogenized alternative to the homogeneous precapture of CO with amines and subsequent hydrogenation to MeOH was developed using aminated silica and a Ru-MACHO catalyst. Commercial mesoporous silica was modified with three different amino-silane monomers and used as support for the Ru catalyst. These composites were studied by TEM and solid-state NMR spectroscopy before and after the catalytic reaction. These catalytic reactions were conducted at 155 °C at a H and CO pressures of 75 and 2 bar, respectively, with the heterogeneous system (gas-solid) being probed with gas-phase infrared spectroscopy used to quantify the resulting products. High turnover number (TON) values were observed for the samples aminated with secondary amines.

摘要

采用氨化硅胶和 Ru-MACHO 催化剂,开发了一种非均相替代方法,用于胺类物质对 CO 的均相预捕获,以及随后的加氢生成甲醇。商业介孔硅胶用三种不同的氨硅烷单体进行改性,用作 Ru 催化剂的载体。在催化反应前后,通过 TEM 和固态 NMR 光谱对这些复合材料进行了研究。这些催化反应在 H 和 CO 的压力分别为 75 和 2 巴的条件下于 155°C 进行,使用气相红外光谱对非均相体系(气-固)进行探测,以定量测定得到的产物。用仲胺进行氨化的样品观察到高的周转数(TON)值。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/605a/10233216/4b33b6dedfc7/OPEN-12-e202300060-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/605a/10233216/c156407b48ca/OPEN-12-e202300060-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/605a/10233216/162dfb0dab65/OPEN-12-e202300060-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/605a/10233216/4b33b6dedfc7/OPEN-12-e202300060-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/605a/10233216/c156407b48ca/OPEN-12-e202300060-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/605a/10233216/162dfb0dab65/OPEN-12-e202300060-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/605a/10233216/4b33b6dedfc7/OPEN-12-e202300060-g003.jpg

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