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首页> 外文期刊>Catalysis science & technology >Additive-free N-methylation of amines with methanol over supported iridium catalyst dagger
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Additive-free N-methylation of amines with methanol over supported iridium catalyst dagger

机译：精细的N-methylation胺甲醇在支持铱催化剂匕首

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摘要

An efficient and versatile zinc oxide-supported iridium (Ir/ZnO) catalyst was developed to catalyze the additive-free N-methylation of amines with methanol. Mechanistic studies suggested that the high catalytic reactivity is rooted in the small sizes (1.4 nm) of Ir nanoparticles and the high ratio (93%) of oxidized iridium species (IrOx, Ir3+ and Ir4+) on the catalyst. Moreover, the delicate cooperation between the IrOx and ZnO support also promoted its high reactivity. The selectivity of this catalytic N-methylation was controllable between dimethylation and monomethylation by carefully tuning the catalyst loading and reaction solvent. Specifically, neat methanol with high catalyst loading (2 mol% Ir) favored the formation of N,N-dimethylated amine, while the mesitylene/methanol mixture with low catalyst loading (0.5 mol% Ir) was prone to producing mono-N-methylated amines. An environmentally benign continuous flow system with a recycled mode was also developed for the efficient production of N-methylated amines. With optimal flow rates and amine concentrations, a variety of N-methylamines were produced with good to excellent yields in this Ir/ZnO-based flow system, providing a starting point for the clean and efficient production of N-methylamines with this cost-effective chemical process.
机译：一种有效的和通用的锌oxide-supported铱(红外/氧化锌)催化剂的开发催化的含添加剂N-methylation胺和甲醇。建议高催化活性基于红外的小尺寸(1.4海里)纳米颗粒和高(93%)的比例氧化铱物种(IrOx Ir3 +和Ir4 +)催化剂。IrOx和氧化锌也支持提升其反应活性高。催化N-methylation之间可控dimethylation和monomethylation小心优化装载催化剂和反应溶剂。具体地说,整洁的甲醇催化剂高加载(2摩尔% Ir)青睐的形成N, N-dimethylated胺,而5 -三甲基苯/甲醇混合较低的催化剂加载(0.5摩尔% Ir)是容易生产mono-N-methylated胺。良性的连续流系统回收模式也为高效开发N-methylated胺的生产。流率和胺的浓度,各种各样的N-methylamines生产好优秀的收益率在这个红外/ ZnO-based流清洁系统,提供了一个起点和高效的生产N-methylamines这有效的化学过程。

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