Fast Isomerization Before Isomerization-Hydroformylation: Probing the Neglected Period with A Novel Microfluidic Device

Guan，Fanfu1; Qian，Yu2; Zhang，Peiqi2; Zhang，Runtong2; Zhang，Xumu2; Wen，Jialin1

2023-05-15

10.1002/anie.202302777

Angewandte Chemie - International Edition   影响因子和分区

1433-7851

1521-3773

By combining the concept of flash chemistry and radial synthesis, a novel microreactor (Flashstop reactor) was designed to study isomerization process of hydroformylation by a Rh/tetraphosphite catalyst in a time scale of seconds. It was found that in the initial 313 seconds, 60–99 % of 1-octene was isomerized to 2- and 3-octenes before the formation of aldehydes. Within this period, two different types of isomerization reactions were observed. It was proposed that a monohydride complex without CO ligand accounts for the ultrafast isomerization in the initial 30 seconds. The isomerization rate with such monohydride species was calculated much faster than that with the well-known H(CO)Rh(P−P) species. Both experimental and DFT computational studies were carried out to support this assumption. Fast transformations early on in catalytic cycles have been rarely studied due to the lack of proper tools. We believe that the Flashstop reactor is a powerful tool for analysis of kinetics in gas-liquid biphasic reactions within a time scale of seconds to minutes.

Fast Kinetics Gas-Liquid Mass Transfer Hydroformylation Isomerization Microfluid Reactor

SCI ; EI

英语

NI论文

通讯

Guangdong Provincial Key Laboratory Of Catalysis[2020B121201002];

Chemistry

Chemistry, Multidisciplinary

WOS:000971937200001

WILEY-V C H VERLAG GMBH

20231713945243

Isomerization ; Isomers ; Mass transfer ; Rhodium compounds

Mass Transfer:641.3 ; Chemical Reactions:802.2 ; Chemical Operations:802.3 ; Chemical Products Generally:804

CHEMISTRY

2-s2.0-85152919860

Scopus

1.Department of Chemical Process R&D,Lianyungang Institute of Research,Jiangsu Hengrui Pharmaceuticals Co.,Ltd.,Lianyungang,7 Kunlunshan Road,222000,China
2.Guangdong Provincial Key Laboratory of Catalysis,Department of Chemistry,Southern University of Science and Technology,Shenzhen,1088 Xueyuan Road,518055,China

Guan，Fanfu,Qian，Yu,Zhang，Peiqi,et al. Fast Isomerization Before Isomerization-Hydroformylation: Probing the Neglected Period with A Novel Microfluidic Device[J]. Angewandte Chemie - International Edition,2023,62(21).

Guan，Fanfu,Qian，Yu,Zhang，Peiqi,Zhang，Runtong,Zhang，Xumu,&Wen，Jialin.(2023).Fast Isomerization Before Isomerization-Hydroformylation: Probing the Neglected Period with A Novel Microfluidic Device.Angewandte Chemie - International Edition,62(21).

Guan，Fanfu,et al."Fast Isomerization Before Isomerization-Hydroformylation: Probing the Neglected Period with A Novel Microfluidic Device".Angewandte Chemie - International Edition 62.21(2023).