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In situ formation of ZnOx species for efficient propane dehydrogenation.

Authors :
Zhao, Dan
Tian, Xinxin
Doronkin, Dmitry E.
Han, Shanlei
Kondratenko, Vita A.
Grunwaldt, Jan-Dierk
Perechodjuk, Anna
Vuong, Thanh Huyen
Rabeah, Jabor
Eckelt, Reinhard
Rodemerck, Uwe
Linke, David
Jiang, Guiyuan
Jiao, Haijun
Kondratenko, Evgenii V.
Source :
Nature; 11/11/2021, Vol. 599 Issue 7884, p234-238, 5p
Publication Year :
2021

Abstract

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. 5–8) 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 ZnO<subscript>x</subscript> 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 ZnO<subscript>x</subscript> species. For benchmarking purposes, the developed ZnO–silicalite-1 and an analogue of commercial K–CrO<subscript>x</subscript>/Al<subscript>2</subscript>O<subscript>3</subscript> 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.Propene is obtained through propane dehydrogenation using catalysts that are toxic, expensive or demanding to regenerate with ecologically harmful compounds, but the ZnO-based alternative reported here is cheap, clean and scalable. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
00280836
Volume :
599
Issue :
7884
Database :
Complementary Index
Journal :
Nature
Publication Type :
Academic Journal
Accession number :
153509891
Full Text :
https://doi.org/10.1038/s41586-021-03923-3