期刊
ACS CATALYSIS
卷 6, 期 4, 页码 2257-2264出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.5b02917
关键词
Pt/gamma-Al2O3; Pt-Sn/gamma-Al2O3; oxidative regeneration; nucleation sites; propane dehydrogenation; sintering; coking; STEM/HRTEM
资金
- Partnership for International Research and Education - National Science Foundation (NSF) [OISE-0730277]
- NSF [EEC-0813570]
- U.S. Department of Energy [DE-FG02-05ER15712]
- Netherlands Research School Combination-Catalysis (NRSC-C)
- European Research Council (ERC) Advanced Grant [321140]
Alumina-supported Pt is one of the major industrial catalysts for light alkane dehydrogenation. This catalyst loses activity during reaction, with coke formation often considered as the reason for deactivation. As we show in this study, the amount and nature of carbon deposits do not directly correlate with the loss of activity. Rather, it is the transformation of subnanometer Pt species into larger Pt nanoparticles that appears to be responsible for the loss of catalytic activity. Surprisingly, a portion of the Sn remains atomically dispersed on the alumina surface in the spent catalyst and helps in the redispersion of the Pt. In the absence of Sn on the alumina support, the larger Pt nanoparticles formed during reaction are not redispersed during oxidative regeneration. It is known that Sn is added as a promoter in the industrial catalyst to help in achieving high propene selectivity and to minimize coke formation. This work shows that an important role of Sn is to help in the regeneration of Pt, by providing nucleation sites on the alumina surface. Aberration-corrected scanning transmission electron microscopy helps to provide unique insights into the operating characteristics of an industrially important catalyst by demonstrating the role of promoter elements, such as Sn, in the oxidative regeneration of Pt on gamma-Al2O3.
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