Thermally Stable and Regenerable Platinum-Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria

被引:340
作者
Xiong, Haifeng [1 ,2 ]
Lin, Sen [3 ]
Goetze, Joris [4 ]
Pletcher, Paul [4 ]
Guo, Hua [5 ]
Kovarik, Libor [6 ]
Artyushkova, Kateryna [1 ,2 ]
Weckhuysen, Bert M. [4 ]
Datye, Abhaya K. [1 ,2 ]
机构
[1] Univ New Mexico, Dept Chem & Biol Engn, Albuquerque, NM 87131 USA
[2] Univ New Mexico, Ctr Microengn Mat, Albuquerque, NM 87131 USA
[3] Fuzhou Univ, State Key Lab Photocatalysis Energy & Environm, Res Inst Photocatalysis, Fuzhou 350002, Fujian, Peoples R China
[4] Univ Utrecht, Inorgan Chem & Catalysis, Debye Inst Nanomat Sci, Univ Weg 99, NL-3584 CG Utrecht, Netherlands
[5] Univ New Mexico, Dept Chem & Chem Biol, Albuquerque, NM 87131 USA
[6] Pacific Northwest Natl Lab, Environm Mol Sci Lab, Richland, WA 99352 USA
基金
美国国家科学基金会; 欧洲研究理事会; 中国国家自然科学基金;
关键词
catalyst regeneration; ceria; light alkane dehydrogenation; single atoms; subnanometer Pt-Sn catalysis; LIGHT ALKANE DEHYDROGENATION; CATALYTIC DEHYDROGENATION; ETHANE DEHYDROGENATION; SUPPORTED PT/SN; SN; NANOPARTICLES; DEACTIVATION; SPECTROSCOPY; ISOBUTANE; PT/AL2O3;
D O I
10.1002/anie.201701115
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Ceria (CeO2) supports are unique in their ability to trap ionic platinum (Pt), providing exceptional stability for isolated single atoms of Pt. The reactivity and stability of single-atom Pt species was explored for the industrially important light alkane dehydrogenation reaction. The single-atom Pt/CeO2 catalysts are stable during propane dehydrogenation, but are not selective for propylene. DFT calculations show strong adsorption of the olefin produced, leading to further unwanted reactions. In contrast, when tin (Sn) is added to CeO2, the single-atom Pt catalyst undergoes an activation phase where it transforms into Pt-Sn clusters under reaction conditions. Formation of small Pt-Sn clusters allows the catalyst to achieve high selectivity towards propylene because of facile desorption of the product. The CeO2-supported Pt-Sn clusters are very stable, even during extended reaction at 680 degrees C. Coke formation is almost completely suppressed by adding water vapor to the feed. Furthermore, upon oxidation the Pt-Sn clusters readily revert to the atomically dispersed species on CeO2, making Pt-Sn/CeO2 a fully regenerable catalyst.
引用
收藏
页码:8986 / 8991
页数:6
相关论文
共 41 条
[1]   FTIR STUDY OF BIMETALLIC PT-SN/AL2O3 CATALYSTS [J].
BALAKRISHNAN, K ;
SCHWANK, J .
JOURNAL OF CATALYSIS, 1992, 138 (02) :491-499
[2]   Propane dehydrogenation over supported Pt and Pt-Sn catalysts: Catalyst preparation, characterization, and activity measurements [J].
Barias, OA ;
Holmen, A ;
Blekkan, EA .
JOURNAL OF CATALYSIS, 1996, 158 (01) :1-12
[3]   Advanced Catalytic Dehydrogenation Technologies for Production of Olefins [J].
Bricker, Jeffery C. .
TOPICS IN CATALYSIS, 2012, 55 (19-20) :1309-1314
[4]  
Bruix A., 2014, ANGEW CHEM, V126, P10693
[5]   Maximum Noble-Metal Efficiency in Catalytic Materials: Atomically Dispersed Surface Platinum [J].
Bruix, Albert ;
Lykhach, Yaroslava ;
Matolinova, Iva ;
Neitzel, Armin ;
Skala, Tomas ;
Tsud, Nataliya ;
Vorokhta, Mykhailo ;
Stetsovych, Vitalii ;
Sevcikova, Klara ;
Myslivecek, Josef ;
Fiala, Roman ;
Vaclavu, Michal ;
Prince, Kevin C. ;
Bruyere, Stephanie ;
Potin, Valerie ;
Illas, Francesc ;
Matolin, Vladimir ;
Libuda, Joerg ;
Neyman, Konstantin M. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (39) :10525-10530
[6]  
Cortright RD, 1996, STUD SURF SCI CATAL, V101, P1185
[7]   Selective dehydrogenation of isobutane over supported Pt/Sn catalysts [J].
Cortright, RD ;
Hill, JM ;
Dumesic, JA .
CATALYSIS TODAY, 2000, 55 (03) :213-223
[8]  
Fung SC, 2001, STUD SURF SCI CATAL, V139, P399
[9]   Propane dehydrogenation over Pt-Cu bimetallic catalysts: the nature of coke deposition and the role of copper [J].
Han, Zhiping ;
Li, Shuirong ;
Jiang, Feng ;
Wang, Tuo ;
Ma, Xinbin ;
Gong, Jinlong .
NANOSCALE, 2014, 6 (17) :10000-10008
[10]   Subnanometer-sized Pt/Sn alloy cluster catalysts for the dehydrogenation of linear alkanes [J].
Hauser, Andreas W. ;
Gomes, Joseph ;
Bajdich, Michal ;
Head-Gordon, Martin ;
Bell, Alexis T. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2013, 15 (47) :20727-20734