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通过水热后处理激活ZrO-WO固体酸催化剂用于傅克反应。

Activation of ZrO-WO solid acid catalysts in a Friedel-Crafts reaction through post-hydrothermal treatment.

作者信息

Li Sha, Yu Ruopeng, Xu Bonan, Wang Zhikun, Wu Chunzheng, Guo Jianzhong

机构信息

Key Laboratory of Chemical Utilization of Forestry Biomass in Zhejiang Province, College of Chemistry and Materials Engineering, Zhejiang A & F University Hangzhou 311300 China

出版信息

RSC Adv. 2022 May 4;12(21):13406-13411. doi: 10.1039/d2ra00519k. eCollection 2022 Apr 28.

Abstract

ZrO-WO mixed oxide plays an essential role in the chemical and petroleum industries. So far, very little work has paid attention to the activation of the low activity of ZrO-WO catalysts. In this work, poorly reactive ZrO-WO was prepared as a model catalyst by a sol-gel method and it was accompanied by post-hydrothermal treatment with various solutions. The catalytic results in the Friedel-Crafts reaction of anisole and benzyl alcohol showed that the post-hydrothermal treatment with ethylenediamine or ammonium hydroxide solutions dramatically improved the activity of ZrO-WO, while the hydrothermal treatments with water or ammonia chloride solution resulted in poorer activity and selectivity. The former treatments were found to induce a huge transformation of the ZrO crystal from monoclinic to tetragonal as well as a significant increase in acidic WO clusters that anchored onto ZrO. The generation of the WO clusters was responsible for the activation of ZrO-WO.

摘要

ZrO-WO混合氧化物在化学工业和石油工业中起着至关重要的作用。到目前为止,很少有工作关注ZrO-WO催化剂低活性的活化。在这项工作中,通过溶胶-凝胶法制备了反应活性较差的ZrO-WO作为模型催化剂,并对其进行了各种溶液的水热后处理。苯甲醚与苯甲醇的傅克反应的催化结果表明,用乙二胺或氢氧化铵溶液进行水热后处理可显著提高ZrO-WO的活性,而用水或氯化铵溶液进行水热处理则导致活性和选择性较差。发现前一种处理可诱导ZrO晶体从单斜晶向四方晶发生巨大转变,以及锚定在ZrO上的酸性WO簇显著增加。WO簇的产生是ZrO-WO活化的原因。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/37d2/9066361/df8452e6c57a/d2ra00519k-f1.jpg

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