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用金/二氧化铈活化分子氧用于木质素模型化合物和有机溶剂木质素的转化。

Activating molecular oxygen with Au/CeO for the conversion of lignin model compounds and organosolv lignin.

作者信息

Song Wu-Lin, Dong Qingmeng, Hong Liang, Tian Zhou-Qi, Tang Li-Na, Hao Wenli, Zhang Hongxi

机构信息

Department of Chemistry and Applied Chemistry, Changji University Changji 831100 Xinjiang China

Product Quality Inspection Institute of Changji Hui Autonomous Prefecture Changji 831100 Xinjiang China.

出版信息

RSC Adv. 2019 Oct 2;9(53):31070-31077. doi: 10.1039/c9ra04838c. eCollection 2019 Sep 26.

Abstract

Au/CeO was demonstrated to be a high efficiency catalyst for the conversion of 2-phenoxyacetophenol (PP-ol) employing O as an oxidant and methyl alcohol as the solvent without using an erosive strong base or acid. Mechanistic investigations, including emission quenching experiments, electron spin-resonance (ESR) and intermediate verification experiments, were carried out. The results verified that the superoxide anion activated by Au/CeO from molecular oxygen plays a vital role in the oxidation of lignin model compounds, and the cleavage of both the β-O-4 and C-C linkages was involved. Au/CeO also performed well in the oxidative conversion of organosolv lignin under mild conditions (453 K), producing vanillin (10.5 wt%), methyl vanillate (6.8 wt%), methylene syringate (3.4 wt%) and a ring-opened product. Based on the detailed characterization data and mechanistic results, Au/CeO was confirmed to be a promising catalytic system.

摘要

Au/CeO被证明是一种高效催化剂,可在不使用腐蚀性强碱或强酸的情况下,以氧气为氧化剂、甲醇为溶剂,将2-苯氧基苯乙酮(PP-ol)进行转化。开展了包括发射猝灭实验、电子自旋共振(ESR)和中间体验证实验在内的机理研究。结果证实,Au/CeO从分子氧中活化的超氧阴离子在木质素模型化合物的氧化中起着至关重要的作用,且涉及β-O-4和C-C键的断裂。Au/CeO在温和条件(453 K)下对有机溶剂木质素的氧化转化也表现良好,生成了香草醛(10.5 wt%)、香草酸甲酯(6.8 wt%)、丁香酸甲酯(3.4 wt%)和一种开环产物。基于详细的表征数据和机理结果,证实Au/CeO是一个有前景的催化体系。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/480e/9072557/d50aff1a2cf5/c9ra04838c-f1.jpg

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