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硅氧烷键中与氧的氢键作用驱动了高硅沸石中伯醇的液相吸附。

Hydrogen bonding to oxygen in siloxane bonds drives liquid phase adsorption of primary alcohols in high-silica zeolites.

作者信息

Radhakrishnan Sambhu, Lejaegere Charlotte, Duerinckx Karel, Lo Wei-Shang, Morais Alysson F, Dom Dirk, Chandran C Vinod, Hermans Ive, Martens Johan A, Breynaert Eric

机构信息

Centre for Surface Chemistry and Catalysis - Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001-Heverlee, Belgium.

NMRCoRe - NMR/X-Ray platform for Convergence Research, KU Leuven, Celestijnenlaan 200F Box 2461, 3001-Heverlee, Belgium.

出版信息

Mater Horiz. 2023 Aug 29;10(9):3702-3711. doi: 10.1039/d3mh00888f.

DOI:10.1039/d3mh00888f
PMID:37401863
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10463557/
Abstract

Upon liquid phase adsorption of C-C primary alcohols on high silica MFI zeolites (Si/Al = 11.5-140), the concentration of adsorbed molecules largely exceeds the concentration of traditional adsorption sites: Brønsted acid and defect sites. Combining quantitative H MAS NMR, qualitative multinuclear NMR and IR spectroscopy, hydrogen bonding of the alcohol function to oxygen atoms of the zeolite siloxane bridges (Si-O-Si) was shown to drive the additional adsorption. This mechanism co-exists with chemi- and physi-sorption on Brønsted acid and defect sites and does not exclude cooperative effects from dispersive interactions.

摘要

在高硅MFI沸石（硅铝比=11.5-140）上进行C-C伯醇的液相吸附时，吸附分子的浓度大大超过传统吸附位点（布朗斯台德酸和缺陷位点）的浓度。结合定量的氢 MAS NMR、定性的多核 NMR 和红外光谱，表明醇官能团与沸石硅氧烷桥（Si-O-Si）的氧原子之间的氢键驱动了额外的吸附。这种机制与在布朗斯台德酸和缺陷位点上的化学吸附和物理吸附共存，并且不排除色散相互作用产生的协同效应。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/44a4/10463557/2ea429b761de/d3mh00888f-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/44a4/10463557/cf22ae822ee4/d3mh00888f-f1.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/44a4/10463557/07cc1615c0ed/d3mh00888f-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/44a4/10463557/2ea429b761de/d3mh00888f-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/44a4/10463557/cf22ae822ee4/d3mh00888f-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/44a4/10463557/371d0961f900/d3mh00888f-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/44a4/10463557/07cc1615c0ed/d3mh00888f-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/44a4/10463557/2ea429b761de/d3mh00888f-f4.jpg

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