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铁钴负载MCM-48的简化合成:用于甲苯选择性液相氧化制苯甲醛的高性能多相催化剂

Streamlined synthesis of iron and cobalt loaded MCM-48: High-performance heterogeneous catalysts for selective liquid-phase oxidation of toluene to benzaldehyde.

作者信息

Kalita Arnab, Talukdar Anup Kumar

机构信息

Department of Chemistry, Gauhati University, Gopinath Bordoloi Nagar, Jalukbari, Guwahati, Assam, 781014, India.

出版信息

Heliyon. 2024 Mar 5;10(6):e27296. doi: 10.1016/j.heliyon.2024.e27296. eCollection 2024 Mar 30.

DOI:10.1016/j.heliyon.2024.e27296
PMID:38510017
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10950511/
Abstract

Hydrothermal synthesis of MCM-48 molecular sieves featuring the incorporation of both iron and cobalt with Si/M ratios of 20, 40 and 80 (where M represents either iron or cobalt) was performed using tetraethyl orthosilicate as the silica source and cetyltrimethylammonium bromide as a template. To gain a comprehensive understanding of the synthesized materials, these were thoroughly characterized using various techniques, including XRD, XPS, UV-Vis (DRS), FT-IR, N adsorption-desorption analysis, SEM with EDX, TEM, TGA and NH-TPD analysis. XRD analysis revealed the presence of well-ordered MCM-48 structure in the metal-incorporated materials, while XPS and UV-Vis DRS confirmed the successful partial incorporation of metal ions precisely in their desired tetrahedral coordination within the framework. To assess their catalytic performance, we studied the activity and selectivity of these catalysts in liquid phase oxidation of toluene using -butyl hydroperoxide as the oxidant. Under optimized conditions, employing a 6% (w/w) Fe-MCM-48 (40) catalyst and maintaining a toluene to oxidant molar ratio of 1:3 at 353 K in a solvent-free environment for 8 h, the oxidation reaction resulted in the formation of benzaldehyde (88.1%) as the major product and benzyl alcohol (11.9%) as the minor product.

摘要

以正硅酸乙酯为硅源、十六烷基三甲基溴化铵为模板剂,水热合成了硅/金属(M,代表铁或钴)比为20、40和80的同时掺入铁和钴的MCM - 48分子筛。为全面了解合成材料,采用多种技术对其进行了深入表征,包括XRD、XPS、UV - Vis(DRS)、FT - IR、N吸附 - 脱附分析、带能谱分析的扫描电子显微镜、透射电子显微镜、热重分析和NH₃ - TPD分析。XRD分析表明,金属掺入材料中存在有序的MCM - 48结构,而XPS和UV - Vis DRS证实金属离子成功地以其所需的四面体配位形式精确地部分掺入骨架中。为评估其催化性能,我们研究了这些催化剂在以叔丁基过氧化氢为氧化剂的甲苯液相氧化反应中的活性和选择性。在优化条件下,使用6%(w/w)的Fe - MCM - 48(40)催化剂,在353 K的无溶剂环境中,保持甲苯与氧化剂的摩尔比为1:3,反应8小时,氧化反应生成苯甲醛(88.1%)为主要产物,苯甲醇(11.9%)为次要产物。

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