In Situ X-Ray Photoelectron Spectroscopy of Model Catalysts: At the Edge of the Gap

被引:103
作者
Blomberg, S. [1 ]
Hoffmann, M. J. [2 ]
Gustafson, J. [1 ]
Martin, N. M. [1 ]
Fernandes, V. R. [3 ]
Borg, A. [3 ]
Liu, Z. [4 ]
Chang, R. [4 ]
Matera, S. [2 ]
Reuter, K. [2 ]
Lundgren, E. [1 ]
机构
[1] Lund Univ, Div Synchrotron Radiat Res, SE-22100 Lund, Sweden
[2] Tech Univ Munich, Dept Chem, D-85747 Garching, Germany
[3] Norwegian Univ Sci & Technol, Dept Phys, NO-7491 Trondheim, Norway
[4] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, ALS, Berkeley, CA 94720 USA
关键词
ROOT-5)R27-DEGREES-O SURFACE OXIDE; PRESSURES; 2; PALLADIUM; PT-GROUP METALS; CO OXIDATION; ULTRAHIGH-VACUUM; PD(100); PLATINUM;
D O I
10.1103/PhysRevLett.110.117601
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
We present high-pressure x-ray photoelectron spectroscopy (HP-XPS) and first-principles kinetic Monte Carlo study addressing the nature of the active surface in CO oxidation over Pd(100). Simultaneously measuring the chemical composition at the surface and in the near-surface gas phase, we reveal both O-covered pristine Pd(100) and a surface oxide as stable, highly active phases in the near-ambient regime accessible to HP-XPS. Surprisingly, no adsorbed CO can be detected during high CO2 production rates, which can be explained by a combination of a remarkably short residence time of the CO molecule on the surface and mass-transfer limitations in the present setup. DOI: 10.1103/PhysRevLett.110.117601
引用
收藏
页数:5
相关论文
共 24 条
[1]   SURFACE CORE-LEVEL SHIFTS AS A PROBE OF THE LOCAL OVERLAYER STRUCTURE - CO ON PD(100) [J].
ANDERSEN, JN ;
QVARFORD, M ;
NYHOLM, R ;
SORENSEN, SL ;
WIGREN, C .
PHYSICAL REVIEW LETTERS, 1991, 67 (20) :2822-2825
[2]   In-situ photoelectron spectroscopy with online activity measurement for catalysis research [J].
Chang, Rui ;
Hong, Young Pyo ;
Axnanda, Stephanus ;
Mao, Baohua ;
Jabeen, Naila ;
Wang, Suidong ;
Tai, Renzhong ;
Liu, Zhi .
CURRENT APPLIED PHYSICS, 2012, 12 (05) :1292-1296
[3]   First principles methods using CASTEP [J].
Clark, SJ ;
Segall, MD ;
Pickard, CJ ;
Hasnip, PJ ;
Probert, MJ ;
Refson, K ;
Payne, MC .
ZEITSCHRIFT FUR KRISTALLOGRAPHIE, 2005, 220 (5-6) :567-570
[4]  
Ertl G., 1997, HDB HETEROGENEOUS CA
[5]   CO Oxidation on Pt-Group Metals from Ultrahigh Vacuum to Near Atmospheric Pressures. 2. Palladium and Platinum [J].
Gao, F. ;
Wang, Y. ;
Cai, Y. ;
Goodman, D. W. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2009, 113 (01) :174-181
[6]   New ambient pressure photoemission endstation at Advanced Light Source beamline 9.3.2 [J].
Grass, Michael E. ;
Karlsson, Patrik G. ;
Aksoy, Funda ;
Lundqvist, Mans ;
Wannberg, Bjorn ;
Mun, Bongjin S. ;
Hussain, Zahid ;
Liu, Zhi .
REVIEW OF SCIENTIFIC INSTRUMENTS, 2010, 81 (05)
[7]   Oscillatory CO oxidation on Pd(100) studied with in situ scanning tunneling microscopy [J].
Hendriksen, BLM ;
Bobaru, SC ;
Frenken, JWM .
SURFACE SCIENCE, 2004, 552 (1-3) :229-242
[8]   The Pd (100)-(√5 x √5)R27°-O surface oxide:: A LEED, DFT and STM study [J].
Kostelnik, Petr ;
Seriani, Nicola ;
Kresse, Georg ;
Mikkelsen, Anders ;
Lundgren, Edvin ;
Blum, Volker ;
Sikola, Tomas ;
Varga, Peter ;
Schmid, Michael .
SURFACE SCIENCE, 2007, 601 (06) :1574-1581
[9]  
Logan D., 1992, J. Catal, V133, P179
[10]   Kinetic hindrance during the initial oxidation of Pd(100) at ambient pressures [J].
Lundgren, E ;
Gustafson, J ;
Mikkelsen, A ;
Andersen, JN ;
Stierle, A ;
Dosch, H ;
Todorova, M ;
Rogal, J ;
Reuter, K ;
Scheffler, M .
PHYSICAL REVIEW LETTERS, 2004, 92 (04) :4-461014