AbstractNonoxidative dehydrogenation of propane is useful for the high selectivity to propylene but is suffering from the heavy coke deposition on the catalyst surface. Herein, we present a proof‐of‐concept application of a hole‐hydrogen (H) couple on a metallic cobalt surface to decrease the deactivation rate. The coupled H atoms on the Cobalt (Co) surface, partially resulting from propane dehydrogenation, enabled the desorption of propylene to avoid deep hydrogenolysis and coke deposition and realize selective and durable propylene production, while conventional Co metal‐based catalysts do not generate propylene. The optimized hole‐H coupled Co catalyst provided a low deactivation rate (0.0036 h−1) and a high turnover frequency (55.6 h−1) for propylene production with a high propane flux (48 vol.% C3H8 in gas feeds) at 550 °C.
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