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Abstract
Propane dehydrogenation is actively pursued as a promising method for propylene production to fill a growing supply-demand gap. As limited by the thermodynamics of this transformation, existing approaches face challenges of relatively low conversion and the need for high temperature and low pressure. In this work, we report a photocatalytic approach that enables conversion beyond what can be achieved by conventional thermocatalysis. With sodium decatungstate and cobaloxime pyridine chloride as cooperative photocatalysts, we achieved a new benchmark in propane dehydrogenation of 68.9% conversion and near unity selectivity toward propylene production at room temperature and atmospheric pressure, with hydrogen as the only byproduct. These results prove the concept of dehydrogenating propane for propylene production using light as the key energy input.
Supplementary materials
Title
Supplementary Information
Description
Materials and reagents, synthesis of DT catalysts, procedures for PDH reactions, trapping experiments, computational methods, picture of experimental setup, 1H NMR spectra obtained using TBADT/COPC system, UV-vis spectra of NaDT and TPPDT, typical GC chromatogram obtained after a PDH reaction, measurements of KH of propane and propylene in acetonitrile, oxidative PDH with NaDT and different oxidants, unfavorable transition state
illustrating the poor performance with the oxidative PDH pathway, proposed mechanism, 1H NMR spectra of fresh and spent COPC, reactions of pre-mixed gas mixture, summary of the catalytic data of PDH catalysts.
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