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通过将磺酸基团引入骨架来提高Ru/UiO-66上乙酰丙酸乙酯向γ-戊内酯的转化。

Enhancing the conversion of ethyl levulinate to γ-valerolactone over Ru/UiO-66 by introducing sulfonic groups into the framework.

作者信息

Yang Jie, Huang Wenjuan, Liu Yongsheng, Zhou Tao

机构信息

School of Mathematics and Physics, Shanghai University of Electric Power Shanghai 200090 China

出版信息

RSC Adv. 2018 May 4;8(30):16611-16618. doi: 10.1039/c8ra01314d. eCollection 2018 May 3.

DOI:10.1039/c8ra01314d
PMID:35540507
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9080342/
Abstract

The conversion of ethyl levulinate (EL) to γ-valerolactone (GVL) is an important reaction in biomass conversion. This process undergoes two consecutive reactions: hydrogenation and transesterification of the intermediate compound, ethyl 4-hydroxypentanoate, which are catalyzed by metal nanoparticles and acid sites, respectively. In this study, we explored the catalytic activity of Ru supported on metal organic frameworks aiming to develop efficient metal-acid bifunctional catalysts for this green process. UiO-66 and its analogues with various substituted groups (-SOH, -NH and -NO) were employed in this study. The Ru particle size, oxidation state and reducibility were characterized by TEM, H-TPR, and XPS. The results suggest that the introduction of functional groups reduces the hydrogenation activity of pristine Ru/UiO-66 to various extents. Catalyst modified with -SOH group shows much higher acidic catalytic performance while showing hydrogenation activity towards C[double bond, length as m-dash]O bonds, thus improving the overall transformation of EL to GVL due to the presence of strong Brønsted acid sites.

摘要

乙酰丙酸乙酯（EL）转化为γ-戊内酯（GVL）是生物质转化中的一个重要反应。该过程经历两个连续反应：中间化合物4-羟基戊酸乙酯的氢化反应和酯交换反应，分别由金属纳米颗粒和酸性位点催化。在本研究中，我们探索了负载在金属有机框架上的Ru的催化活性，旨在开发用于这一绿色过程的高效金属-酸双功能催化剂。本研究采用了UiO-66及其具有各种取代基（-SOH、-NH和-NO）的类似物。通过透射电子显微镜（TEM）、氢气程序升温还原（H-TPR）和X射线光电子能谱（XPS）对Ru的粒径、氧化态和还原性能进行了表征。结果表明，官能团的引入在不同程度上降低了原始Ru/UiO-66的氢化活性。用-SOH基团改性的催化剂表现出更高的酸性催化性能，同时对C=O键表现出氢化活性，因此由于存在强布朗斯特酸位点，提高了EL向GVL的整体转化率。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/675a4a90d14d/c8ra01314d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/6dbd46a6367b/c8ra01314d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/2746eb24e416/c8ra01314d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/3c1e7f0aaf8e/c8ra01314d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/612a8f94bc27/c8ra01314d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/675a4a90d14d/c8ra01314d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/6dbd46a6367b/c8ra01314d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/2746eb24e416/c8ra01314d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/3c1e7f0aaf8e/c8ra01314d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/612a8f94bc27/c8ra01314d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8cf6/9080342/675a4a90d14d/c8ra01314d-f5.jpg

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