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Peroxotungstate-Based Ionic Hybrid as a Triphase Heterogeneous Catalyst for Efficient Benzyl Alcohol Oxidation Under Mild Conditions
Catalysis Letters ( IF 2.3 ) Pub Date : 2019-12-20 , DOI: 10.1007/s10562-019-03071-4
Manman Jin , Qingtao Niu , Chongdian Si , Zhiguo Lv , Hongyue Guo , Zhenmei Guo

Abstract Supported ionic-liquid-phases (SILPs) were synthesized via reaction of 1-methyl-3-(3-triethoxysilylpropyl)imidazolium hexafluorophosphate (ImCl-PF 6 ) with SBA-15 and then peroxotungstate molecules were immobilized on SILPs. The resulting material (W-ImCl-PF 6 -SBA-15) was characterized via 29 Si MAS NMR to detect the chemical environment around Si and its textural and thermogravimetric behavior were determined. To obtain insight into the role of ImCl-PF 6 during catalysis, an ImCl-PF 6 -free catalyst (W/SBA-15) was also synthesized. W-ImCl-PF 6 -SBA-15 and W/SBA-15 were investigated as catalysts for benzyl alcohol oxidation, as a model reaction, under solvent-free conditions with H 2 O 2 .The presence of ImCl-PF 6 was crucial for obtaining excellent catalytic activity, and W-ImCl-PF 6 -SBA-15 showed higher activity and stability than these of W/SBA-15. Optimized reaction conditions were employed to several selected alcohols oxidation and, remarkably, excellent aldehydes selectivity was achieved. The importance of ImCl-PF 6 -functionalized SBA-15 was evidenced via recycling experiments of benzyl alcohol oxidation, and W-ImCl-PF 6 -SBA-15 was recycled for ten reaction runs without significant change in benzyl alcohol conversion, benzaldehyde selectivity, and tungsten content. Graphic Abstract

中文翻译:

基于过氧钨酸盐的离子杂化物作为三相多相催化剂在温和条件下有效氧化苯甲醇

摘要 通过1-甲基-3-(3-三乙氧基甲硅烷基丙基)咪唑鎓六氟磷酸盐(ImCl-PF 6 )与SBA-15反应合成负载型离子液相(SILPs),然后将过氧钨酸盐分子固定在SILPs上。所得材料 (W-ImCl-PF 6 -SBA-15) 通过 29 Si MAS NMR 进行表征,以检测 Si 周围的化学环境,并确定其结构和热重行为。为了深入了解 ImCl-PF 6 在催化过程中的作用,还合成了一种不含 ImCl-PF 6 的催化剂 (W/SBA-15)。W-ImCl-PF 6 -SBA-15 和 W/SBA-15 作为苯甲醇氧化的催化剂,作为模型反应,在无溶剂条件下与 H 2 O 2 进行了研究。ImCl-PF 6 的存在是至关重要的为了获得优异的催化活性,W-ImCl-PF 6 -SBA-15 显示出比 W/SBA-15 更高的活性和稳定性。优化的反应条件用于几种选定的醇氧化,并且显着地实现了优异的醛选择性。ImCl-PF 6 -官能化的 SBA-15 的重要性通过苯甲醇氧化的循环实验得到证实,并且 W-ImCl-PF 6 -SBA-15 循环十次反应运行,苯甲醇转化率、苯甲醛选择性、和钨含量。图形摘要 并且 W-ImCl-PF 6 -SBA-15 被循环用于十次反应运行,而苯甲醇转化率、苯甲醛选择性和钨含量没有显着变化。图形摘要 并且 W-ImCl-PF 6 -SBA-15 被循环用于十次反应运行,而苯甲醇转化率、苯甲醛选择性和钨含量没有显着变化。图形摘要
更新日期:2019-12-20
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