Maximum Noble-Metal Efficiency in Catalytic Materials: Atomically Dispersed Surface Platinum

被引:398
作者
Bruix, Albert [1 ,2 ]
Lykhach, Yaroslava [4 ]
Matolinova, Iva [6 ]
Neitzel, Armin [4 ]
Skala, Tomas [6 ]
Tsud, Nataliya [6 ]
Vorokhta, Mykhailo [6 ]
Stetsovych, Vitalii [6 ]
Sevcikova, Klara [6 ]
Myslivecek, Josef [6 ]
Fiala, Roman [6 ]
Vaclavu, Michal [6 ]
Prince, Kevin C. [8 ,9 ]
Bruyere, Stephanie [7 ]
Potin, Valerie [7 ]
Illas, Francesc [1 ,2 ]
Matolin, Vladimir [6 ]
Libuda, Joerg [4 ,5 ]
Neyman, Konstantin M. [1 ,2 ,3 ]
机构
[1] Univ Barcelona, Dept Quim Fis, E-08028 Barcelona, Spain
[2] Univ Barcelona, Inst Quim Teor & Computac IQTCUB, E-08028 Barcelona, Spain
[3] ICREA, Barcelona 08010, Spain
[4] Univ Erlangen Nurnberg, Lehrstuhl Phys Chem 2, Erlangen, Germany
[5] Univ Erlangen Nurnberg, Erlangen Catalysis Resource Ctr, D-91058 Erlangen, Germany
[6] Charles Univ Prague, Dept Surface & Plasma Sci, CR-18000 Prague, Czech Republic
[7] Univ Bourgogne, CNRS, Lab Interdisciplinaire Carnot Bourgogne, UMR 6303, F-21078 Dijon, France
[8] Sincrotrone Trieste SCpA, I-34149 Basovizza Trieste, Italy
[9] IOM, I-34149 Basovizza Trieste, Italy
关键词
ceria nanoparticles; density functional calculations; heterogeneous catalysis; model catalyst; platinum; CERIA NANOPARTICLES; OXYGEN REDUCTION; ATOMS; OXIDE; SIZE; MECHANISM;
D O I
10.1002/anie.201402342
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Platinum is the most versatile element in catalysis, but it is rare and its high price limits large-scale applications, for example in fuel-cell technology. Still, conventional catalysts use only a small fraction of the Pt content, that is, those atoms located at the catalyst's surface. To maximize the noble-metal efficiency, the precious metal should be atomically dispersed and exclusively located within the outermost surface layer of the material. Such atomically dispersed Pt surface species can indeed be prepared with exceptionally high stability. Using DFT calculations we identify a specific structural element, a ceria "nanopocket", which binds Pt2+ so strongly that it withstands sintering and bulk diffusion. On model catalysts we experimentally confirm the theoretically predicted stability, and on real Pt-CeO2 nanocomposites showing high Pt efficiency in fuel-cell catalysis we also identify these anchoring sites.
引用
收藏
页码:10525 / 10530
页数:6
相关论文
共 40 条
[1]  
Armstrong G., 2013, NAT CHEM, V5, P809
[2]   Relative Stabilities of Low Index and Stepped CeO2 Surfaces from Hybrid and GGA plus U Implementations of Density Functional Theory [J].
Branda, Maria M. ;
Ferullo, Ricardo M. ;
Causa, Mauro ;
Illas, Francesc .
JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (09) :3716-3721
[3]   On the adsorption and formation of Pt dimers on the CeO2(111) surface [J].
Bruix, Albert ;
Nazari, Fariba ;
Neyman, Konstantin M. ;
Illas, Francesc .
JOURNAL OF CHEMICAL PHYSICS, 2011, 135 (24)
[4]   Adsorption, Oxidation State, and Diffusion of Pt Atoms on the CeO2(111) Surface [J].
Bruix, Albert ;
Neyman, Konstantin M. ;
Illas, Francesc .
JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (33) :14202-14207
[5]   Control of Metal Nanocrystal Size Reveals Metal-Support Interface Role for Ceria Catalysts [J].
Cargnello, Matteo ;
Doan-Nguyen, Vicky V. T. ;
Gordon, Thomas R. ;
Diaz, Rosa E. ;
Stach, Eric A. ;
Gorte, Raymond J. ;
Fornasiero, Paolo ;
Murray, Christopher B. .
SCIENCE, 2013, 341 (6147) :771-773
[6]   Active and stable carbon nanotube/nanoparticle composite electrocatalyst for oxygen reduction [J].
Chung, Hoon T. ;
Won, Jong H. ;
Zelenay, Piotr .
NATURE COMMUNICATIONS, 2013, 4
[7]  
Cotton F. A., 1990, ADV INORGANIC CHEM
[8]  
ERTL G, 2008, ANGEW CHEM, V120, P3578, DOI DOI 10.1002/ANGE.200800480
[9]  
Ertl G., 2008, Handbook of Heterogeneous Catalysis, V1, DOI DOI 10.1002/9783527610044.HETCAT0130
[10]   Reactions at surfaces: From atoms to complexity (Nobel lecture) [J].
Ertl, Gerhard .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (19) :3524-3535