Modification of Cs/SiO2 with Zr element through sol–gel method for production of methyl methacrylate via one-step aldol condensation

IF 4.1 2区工程技术 Q2 ENGINEERING, CHEMICAL

Chemical Engineering Science Pub Date : 2024-11-04 DOI:10.1016/j.ces.2024.120899

Jinguo Hao , Junyang Liu , Senlin Deng , Lei Wang , Gang Wang , Chunshan Li

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引用次数: 0

Abstract

Development of effective cesium-based catalyst is important for methyl methacrylate (MMA) production via one-step aldol reaction. Herein, a kind of Cs/Zr-SiO₂ catalyst was prepared by sol–gel method and the acid-base properties and their balance could be controllably regulated. The influence of catalyst preparation conditions including Si/Zr ratio and water content on the structure and acid-base properties of Cs/Zr-SiO₂ was demonstrated, which consequentially affected catalytic performance. The formation of Si-O-Zr and Cs-O-Si structure was identified as the dominant Lewis acid and base sites and the acid site density can be enhanced by 1-fold when using sol–gel method. In addition, the MP conversion could reach 37 % with MMA selectivity of 85 % at the optimal condition. Kinetic studies revealed that the activation barrier on the modified 10Cs/Zr-SiO₂ exhibited the lowest activation energy of 110.9 kJ/mol. Besides, the initial catalytic activity could still maintain after 800 h recycling, with single-pass life of 160 h.

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通过溶胶-凝胶法用 Zr 元素改性 Cs/SiO2 以通过一步醛醇缩合法生产甲基丙烯酸甲酯

开发有效的铯基催化剂对于通过一步醛醇反应生产甲基丙烯酸甲酯（MMA）非常重要。本文采用溶胶-凝胶法制备了一种 Cs/Zr-SiO2 催化剂，并对其酸碱性质及其平衡进行了可控调节。结果表明，Si/Zr比和含水量等催化剂制备条件对Cs/Zr-SiO2的结构和酸碱性质有影响，进而影响催化性能。在溶胶-凝胶法中，Si-O-Zr 和 Cs-O-Si 结构的形成被确定为主要的路易斯酸和碱位点，酸位点密度可提高 1 倍。此外，在最佳条件下，MP 转化率可达 37%，MMA 选择性为 85%。动力学研究表明，改性 10Cs/Zr-SiO2 的活化能最低，为 110.9 kJ/mol。此外，在循环使用 800 小时后仍能保持初始催化活性，单次使用时间为 160 小时。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Chemical Engineering Science 工程技术-工程：化工

CiteScore

7.50

自引率

8.50%

发文量

1025

审稿时长

50 days

期刊介绍： Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline. Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.