TiO2-Supported catalysts with ZnO and ZrO2for non-oxidative dehydrogenation of propane: mechanistic analysis and application potential

被引:15
作者
Han, Shanlei [1 ,2 ]
Zhao, Dan [1 ,2 ]
Lund, Henrik [1 ]
Rockstroh, Nils [1 ]
Bartling, Stephan [1 ]
Doronkin, Dmitry E. [3 ,4 ]
Grunwaldt, Jan-Dierk [3 ,4 ]
Gao, Manglai [2 ]
Jiang, Guiyuan [2 ]
Kondratenko, Evgenii V. [1 ]
机构
[1] Leibniz Inst Katalyse eV, Albert Einstein Str 29 A, D-18059 Rostock, Germany
[2] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
[3] Karlsruhe Inst Technol KIT, Inst Catalysis Res & Technol, Kaiserstr 12, D-76131 Karlsruhe, Germany
[4] Karlsruhe Inst Technol KIT, Inst Chem Technol & Polymer Chem, Kaiserstr 12, D-76131 Karlsruhe, Germany
基金
中国国家自然科学基金;
关键词
OXIDATIVE DEHYDROGENATION; METHANOL CONVERSION; LOW-TEMPERATURE; CO; SELECTIVITY; CHEMISTRY; PLATINUM; ETHANE; SITE; HYDROGENATION;
D O I
10.1039/d0cy01416h
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Non-oxidative dehydrogenation of propane is one of the most promising technologies for propene production in terms of environmental impact and sustainability. The purpose of the present study was to develop environmentally friendly and low-cost alternatives to currently applied Pt- or CrOx-based catalysts. Rutile TiO2-based catalysts with supported ZnO(x)and ZrO(x)species were established to show promising performance under industrially relevant conditions. The amount of propene produced within 3 h on propane stream at 550 degrees C over the optimized catalyst with 2 wt% Zn and 5.6 wt% Zr is close to that obtained over commercial-like K-CrOx/Al(2)O(3)and the state-of-the-art Cu/YZrO(x)catalyst. The selectivity to propene over our catalyst was about 95% at a propane conversion of about 23%. The kind of active sites and the effect of ZrO(2)addition on catalyst performance and physicochemical properties were elucidated owing to the application of complementary characterisation techniques such as XRD, N(2)physisorption, HRTEM, EDX, XPS, X-ray absorption spectroscopy, NH3-TPD, CO-TPR, Raman and O-2-TPO. ZnO(x)clusters with 1-3 Zn atoms were concluded to be the active sites. ZrO(2)enhances their intrinsic activity and inhibits the formation of the inactive rhombohedral ZnTiO(3)phase.
引用
收藏
页码:7046 / 7055
页数:10
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