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Selective Oxidation of Benzylic sp<sup>3</sup> C–H Bonds using Molecular Oxygen in a Continuous-Flow Microreactor

Lei Yun, Jingnan Zhao, Xiaofei Tang, Cunfei Ma, Zongyi Yu, Qingwei Meng

2021Organic Process Research & Development22 citationsDOI

Abstract

Selective aerobic oxidation of benzylic sp3 C–H bonds to generate the corresponding ketones was achieved under continuous-flow conditions. The catalysts N-hydroxyphthalimide (NHPI) and tert-butyl nitrite (TBN) as the precursor of the radical under aerobic conditions motivated this process. Flow microreactors operating under optimized conditions enabled this oxidation with higher efficiency and a shortened reaction time of 54 s (total time was 10 min), which was improved 466 times compared with the batch parallel reaction (7.0 h). Notably, the catalyst and solvent recycling (92.6 and 94.5%) and scale-up experiments (0.87 g h–1 in 28 h) demonstrated the practicability of the protocol. The high product selectivity and functional group tolerance of the process allowed the production of ketones in yields of 41.2 to 90.3%. To reveal the versatility and applicability of this protocol, the late-stage modification of an antiepileptic drug to obtain oxcarbazepine was further conducted.

Topics & Concepts

MicroreactorChemistryCatalysisSelectivityContinuous flowSolventMolecular oxygenFunctional groupOxidation processCombinatorial chemistryOrganic chemistryChemical engineeringPhysicsPolymerMechanicsEngineeringOxidative Organic Chemistry ReactionsInnovative Microfluidic and Catalytic Techniques InnovationRadical Photochemical Reactions
Selective Oxidation of Benzylic sp<sup>3</sup> C–H Bonds using Molecular Oxygen in a Continuous-Flow Microreactor | Litcius