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Tandem Catalytic Amine Synthesis from Alkenes in Continuous Flow Enabled by Integrated Catalyst Recycling
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-05-11 , DOI: 10.1021/acscatal.0c01465 Jonas Bianga 1 , Kai U. Künnemann 1 , Lisa Goclik 1 , Lasse Schurm 1 , Dieter Vogt 1 , Thomas Seidensticker 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-05-11 , DOI: 10.1021/acscatal.0c01465 Jonas Bianga 1 , Kai U. Künnemann 1 , Lisa Goclik 1 , Lasse Schurm 1 , Dieter Vogt 1 , Thomas Seidensticker 1
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We present the development of catalytic autotandem reactions into continuous-flow processes on the example of homogeneously catalyzed hydroaminomethylation (consisting of hydroformylation and subsequent reductive amination) as a case study. The synthesis of higher aliphatic amines was successfully operated in a continuous-flow miniplant. Key to success was the development of an integrated catalyst recycling for the homogeneous Rhodium/SulfoXantphos catalyst. With 1-decene and diethylamine as substrates, an average yield of the linear amine of 61% over 60 h of stable process operation was achieved. The catalyst recycling has been accomplished by using a thermomorphic multiphase system (TMS) consisting of methanol and n-dodecane, which was rationally established in batch experiments with a methodical approach. This TMS ensured high catalytic activities and facilitated an efficient catalyst separation and recycling. Before application in a continuous process, catalyst recyclability was proven, showing high catalyst activity over six runs with turnover frequencies up to 2400 h–1.
中文翻译：
集成催化剂回收技术在连续流动条件下由烯烃串联催化合成胺
我们以均相催化的氢氨基甲基化（由加氢甲酰基化和随后的还原胺化反应为例）为例，介绍催化自串联反应向连续流过程的发展。高级脂族胺的合成已在连续流微型设备中成功进行。成功的关键是开发用于均相铑/磺基黄磷催化剂的集成催化剂回收系统。以1-癸烯和二乙胺为底物，在稳定的工艺操作60小时内，线性胺的平均收率达到61％。所述催化剂的回收已经通过使用一个thermomorphic多相系统（TMS）由甲醇和完成Ñ-十二烷，这是在批量实验中采用系统方法合理建立的。该TMS确保了高催化活性，并促进了有效的催化剂分离和再循环。在应用于连续过程之前，已证明了催化剂的可回收性，在六次运行中显示出高催化剂活性，周转频率高达2400 h –1。
更新日期：2020-05-11
中文翻译：
集成催化剂回收技术在连续流动条件下由烯烃串联催化合成胺
我们以均相催化的氢氨基甲基化（由加氢甲酰基化和随后的还原胺化反应为例）为例，介绍催化自串联反应向连续流过程的发展。高级脂族胺的合成已在连续流微型设备中成功进行。成功的关键是开发用于均相铑/磺基黄磷催化剂的集成催化剂回收系统。以1-癸烯和二乙胺为底物，在稳定的工艺操作60小时内，线性胺的平均收率达到61％。所述催化剂的回收已经通过使用一个thermomorphic多相系统（TMS）由甲醇和完成Ñ-十二烷，这是在批量实验中采用系统方法合理建立的。该TMS确保了高催化活性，并促进了有效的催化剂分离和再循环。在应用于连续过程之前，已证明了催化剂的可回收性，在六次运行中显示出高催化剂活性，周转频率高达2400 h –1。
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