Spatially isolated cobalt oxide sites derived from MOFs for direct propane dehydrogenation
2021
Wang, Yansu | Suo, Yujun | Ren, Jin-Tao | Wang, Zheng | Yuan, Zhong-Yong
The “active site isolation” strategy has been proved to be efficient for enhancing the catalytic performance in propane dehydrogenation (PDH). Herein, spatially isolated cobalt oxide sites within nitrogen-doped carbon (NC) layers supported on silicalite-1 zeolite (CoOₓ@NC/S-1) were synthesized by a two-step process consisting of the pyrolysis of bimetallic Zn/Co zeolitic imidazole frameworks loaded on silicalite-1 (ZnCo-ZIF/S-1) under N₂ and the subsequent calcination in air atmosphere. This catalyst possesses exceptional catalytic performance for PDH with the propane conversion of 40% and the propene selectivity of >97%, and no apparent deactivation is observed after 10 h PDH reaction at 600 °C. With intensive characterizations and experiments, it is indicated that the real active sites of CoOₓ@NC/S-1 are isolated CoO sites during the PDH process. In situ FT-IR spectroscopy shows the same intermediate product (Co-C₃H₇) during both propane dehydrogenation and propene hydrogenation, indicating that they have a reverse reaction process, and a reaction mechanism for PDH is proposed accordingly.
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