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In situ formation of ZnOx species for efficient propane dehydrogenation
Nature  (IF49.962),  Pub Date : 2021-11-10, DOI: 10.1038/s41586-021-03923-3
Dan Zhao, Xinxin Tian, Dmitry E. Doronkin, Shanlei Han, Vita A. Kondratenko, Jan-Dierk Grunwaldt, Anna Perechodjuk, Thanh Huyen Vuong, Jabor Rabeah, Reinhard Eckelt, Uwe Rodemerck, David Linke, Guiyuan Jiang, Haijun Jiao, Evgenii V. Kondratenko

Propane dehydrogenation (PDH) to propene is an important alternative to oil-based cracking processes, to produce this industrially important platform chemical1,2. The commercial PDH technologies utilizing Cr-containing (refs. 3,4) or Pt-containing (refs. 5,6,7,8) catalysts suffer from the toxicity of Cr(vi) compounds or the need to use ecologically harmful chlorine for catalyst regeneration9. Here, we introduce a method for preparation of environmentally compatible supported catalysts based on commercial ZnO. This metal oxide and a support (zeolite or common metal oxide) are used as a physical mixture or in the form of two layers with ZnO as the upstream layer. Supported ZnOx species are in situ formed through a reaction of support OH groups with Zn atoms generated from ZnO upon reductive treatment above 550 °C. Using different complementary characterization methods, we identify the decisive role of defective OH groups for the formation of active ZnOx species. For benchmarking purposes, the developed ZnO–silicalite-1 and an analogue of commercial K–CrOx/Al2O3 were tested in the same setup under industrially relevant conditions at close propane conversion over about 400 h on propane stream. The developed catalyst reveals about three times higher propene productivity at similar propene selectivity.