水对活性MgAl水滑石活性和稳定性的影响

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Yuanzhou Xi, Robert J. Davis
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引用次数: 96

摘要

采用共沉淀法合成了镁铝摩尔比为4的镁铝水滑石。利用Mg-Al水滑石热分解再水化,在333 K下催化模型甘油三酯三丁酸酯与甲醇(三丁酸∶甲醇摩尔比1:30)酯交换反应,生成丁酸甲酯、单丁酸甲酯、二丁酸甲酯和甘油。通过对实验数据拟合动力学模型,确定了三丁酸甘油酯酯交换三步反应序列的准一级速率常数。通过N2吸附测定的Mg-Al水滑石比分解后的Mg-Al水滑石的表面积要高一个数量级,但活性与CO2吸附能力密切相关。最活跃的再水合样品也更快地失活,可能是因为酯与吸附的水水解产生的丁酸与碱基发生了反应。随着加热去除层间水,Mg-Al水滑石的表面积速率和CO2吸附能力下降。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Influence of water on the activity and stability of activated MgAl hydrotalcites for the transesterification of tributyrin with methanol

Magnesium–aluminum hydrotalcite with a Mg/Al molar ratio of 4 was synthesized by a coprecipitation method. Thermally-decomposed and rehydrated Mg–Al hydrotalcites were used to catalyze the transesterification of tributyrin, a model triglyceride, with methanol (tributyrin:methanol molar ratio 1:30) at 333 K to produce methyl butyrate, monobutyrin, dibutyrin, and glycerol. The pseudo first order rate constants of a three step reaction sequence for tributyrin transesterification were determined by fitting a kinetic model to the experimental data. Although decomposed and rehydrated Mg–Al hydrotalcite was one order of magnitude more active than decomposed Mg–Al hydrotalcite based on surface area measured by N2 adsorption, the activity correlated well to the CO2 adsorption capacity. The most active rehydrated samples also deactivated faster, presumably because butyric acid produced by hydrolysis of ester with adsorbed water reacted with the base sites. The areal rate and CO2 adsorption capacity of decomposed-rehydrated Mg–Al hydrotalcite decreased as the interlayer water was removed by heating.

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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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