Mechanistic study of heterogeneous multifunctional catalytic systems is crucial, but remains challenging, for understanding and improving catalyst performance. Here, we demonstrate that a thorough mechanistic study of a multistep reaction can guide the controllable synthesis of tetrahydroquinolines and quinolines. The one-pot production can be achieved, catalyzed by bifunctional metal-organic framework-supported Pd nanoparticles. Our study identifies a reaction network of six intermediates and ten transformation steps from both ex situ study and operando magic angle spinning NMR spectroscopy under high-pressure H2. In particular, multiple reactive intermediates were detected in high concentrations, unobserved with conventional chromatographic techniques. The molecular-level understanding of the reaction network enables the kinetic control of the conversions of intermediates with an additional cooperative active site, to achieve selective production of products on demand.

Deciphering complex reaction network for selectively switching conversion products with metal-organic framework-supported Pd tandem catalysts

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.