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镁/十六烷基三甲基溴化铵比例对非晶态介孔硅酸镁催化剂的结构、物理化学性质及催化活性的影响

Influence of Mg/CTAB ratio on the structural, physicochemical properties and catalytic activity of amorphous mesoporous magnesium silicate catalysts.

作者信息

Tan Kok-Hou, Iqbal Anwar, Adam Farook, Abu Bakar N H H, Ahmad M N, Yusop Rahimi M, Pauzi Hariy

机构信息

School of Chemical Sciences, Universiti Sains Malaysia 11800 Penang Malaysia

School of Chemical Sciences and Food Technology, Faculty of Science and Technology, Universiti Kebangsaan Malaysia 43600 UKM, Bangi Malaysia.

出版信息

RSC Adv. 2019 Nov 26;9(66):38760-38771. doi: 10.1039/c9ra08024d. eCollection 2019 Nov 25.

DOI:10.1039/c9ra08024d
PMID:35540239
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9075996/
Abstract

This study investigated the physicochemical and catalytic properties of mesoporous magnesium silicate catalysts prepared at various Mg/CTAB ratios (0.25, 0.50, 0.75 and 1.00). The XPS analysis detected a mixture of enstatite and magnesium carbonate species when the Mg/CTAB ratio was 0.25, and 0.50. A mixture of forsterite and magnesium carbonate species were detected when the Mg/CTAB ratio was 0.75 whereas for the Mg/CTAB ratio of 1.00, enstatite and magnesium metasilicate species were detected. A catalyst with the Mg/CTAB ratio of 1.00 demonstrated the highest catalytic activity in the oxidation of styrene. The styrene conversion rate was 59.0%, with 69.2% styrene oxide (StO) selectivity. The HO molecules were activated regio-specifically by the magnesium species to prevent rapid self-decomposition while promoting selective interaction with styrene. All the parameters that influence the styrene conversion and product selectivity were evaluated using analysis of variance (ANOVA) with Tukey's test. The ANOVA analysis showed that the reaction time (h), Mg/CTAB ratio, styrene/HO ratio, catalyst loading (mg) and temperature (°C) affect styrene conversion and product selectivity (StO) significantly ( < 0.05). The oxidation of styrene was well fitted to the pseudo-first-order model. The activation energy, of the catalysed styrene epoxidation reaction was calculated to be 27.7 kJmol. The catalyst can be reused several times without any significant loss in its activity and selectivity. The results from this study will be useful in designing and developing low cost, high activity catalysts from alkaline earth metals.

摘要

本研究考察了在不同Mg/CTAB比例(0.25、0.50、0.75和1.00)下制备的介孔硅酸镁催化剂的物理化学性质和催化性能。XPS分析检测到,当Mg/CTAB比例为0.25和0.50时,存在顽火辉石和碳酸镁物种的混合物。当Mg/CTAB比例为0.75时,检测到镁橄榄石和碳酸镁物种的混合物,而当Mg/CTAB比例为1.00时,检测到顽火辉石和偏硅酸镁物种。Mg/CTAB比例为1.00的催化剂在苯乙烯氧化反应中表现出最高的催化活性。苯乙烯转化率为59.0%,环氧苯乙烯(StO)选择性为69.2%。HO分子被镁物种区域特异性活化,以防止快速自分解,同时促进与苯乙烯的选择性相互作用。使用方差分析(ANOVA)和Tukey检验评估了所有影响苯乙烯转化率和产物选择性的参数。方差分析表明,反应时间(h)、Mg/CTAB比例、苯乙烯/HO比例、催化剂负载量(mg)和温度(°C)对苯乙烯转化率和产物选择性(StO)有显著影响(<0.05)。苯乙烯氧化反应很好地符合准一级模型。催化苯乙烯环氧化反应的活化能计算为27.7 kJmol。该催化剂可以重复使用多次,其活性和选择性没有任何显著损失。本研究结果将有助于设计和开发低成本、高活性的碱土金属催化剂。

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