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使用不同方法在纳米结构KIT-6中生成酸性位点以获得用于甘油缩醛化制备丙酮缩甘油的高效酸性催化剂。

Generation of Acid Sites in Nanostructured KIT-6 Using Different Methods to Obtain Efficient Acidic Catalysts for Glycerol Acetalization to Solketal.

作者信息

Janiszewska Ewa, Kowalska-Kuś Jolanta, Wiktorowska Justyna, Jankowska Aldona, Tabero Agata, Held Agnieszka, Kowalak Stanisław

机构信息

Faculty of Chemistry, Adam Mickiewicz University, Uniwersytetu Poznańskiego 8, 61-614 Poznań, Poland.

出版信息

Molecules. 2024 Nov 21;29(23):5512. doi: 10.3390/molecules29235512.

Abstract

This study explored the preparation of pure silica KIT-6, as well as KIT-6 materials with an enhanced concentration of surface OH groups through aluminum incorporation or NHF treatment. These materials with various contents of surface OH groups were subsequently modified via the post-synthesis grafting of sulfonic groups using 3-mercaptopropyltrimethoxysilane as a precursor, followed by oxidation to introduce acidic sites. The catalysts were thoroughly characterized using XRD, nitrogen adsorption/desorption, SEM-EDS, TEM, and FT-IR techniques to confirm their structural and chemical properties. The catalytic activity of acid-functionalized mesoporous silicas of the KIT-6 structure was further evaluated in the acetalization of glycerol to produce solketal. The results demonstrated a significant influence of the surface OH group concentration and acidic site density on catalytic performance, with KIT-6_F_SOH showing the highest efficiency in glycerol-to-solketal conversion. This study provides valuable insights into the design of efficient catalytic systems for the valorization of biodiesel-derived glycerol into high-value chemicals, offering a sustainable approach to waste glycerol utilization.

摘要

本研究探索了纯二氧化硅KIT-6以及通过引入铝或进行NHF处理来提高表面羟基浓度的KIT-6材料的制备方法。随后,使用3-巯丙基三甲氧基硅烷作为前体,通过后合成接枝磺酸基团对这些具有不同表面羟基含量的材料进行改性,然后氧化以引入酸性位点。使用XRD、氮吸附/脱附、SEM-EDS、TEM和FT-IR技术对催化剂进行了全面表征,以确认其结构和化学性质。进一步评估了KIT-6结构的酸功能化介孔二氧化硅在甘油缩醛化制备丙酮缩甘油中的催化活性。结果表明,表面羟基浓度和酸性位点密度对催化性能有显著影响,其中KIT-6_F_SOH在甘油转化为丙酮缩甘油的过程中表现出最高效率。本研究为设计将生物柴油衍生甘油转化为高价值化学品的高效催化系统提供了有价值的见解,为废甘油的利用提供了一种可持续的方法。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ef39/11643615/63939a716cf8/molecules-29-05512-g001.jpg

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