Carbon Dissolution and Segregation in Pd(110)

被引:21
作者
Bowker, Michael [1 ]
Counsell, Jonathan [1 ]
El-Abiary, Kareem [1 ]
Gilbert, Lee [1 ]
Morgan, Chris [1 ]
Nagarajan, Sankaranarayanan [2 ]
Gopinath, Chinnakonda S. [2 ]
机构
[1] Cardiff Univ, Sch Chem, Wolfson Nanosci Lab, Cardiff CF10 3AT, S Glam, Wales
[2] Natl Chem Lab, Catalysis Div, Pune 411008, Maharashtra, India
基金
英国工程与自然科学研究理事会;
关键词
VINYL-ACETATE SYNTHESIS; MOLECULAR-BEAM; ETHENE OXIDATION; ACETIC-ACID; ADSORPTION; PALLADIUM; SURFACE; PD; DECOMPOSITION; KINETICS;
D O I
10.1021/jp9108046
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
The bulk-surface diffusion of carbon in Pd(110) has been investigated using Molecular beams to examine the clean-off of carbon with gas-phase oxygen. The dominant product of the reaction above 600 K is CO CO, is only produced at much lower temperatures where the lifetime of adsorbed CO is significant. The segregation from the bulk Only Occurs at a measurable rate at >750 K, while loss of carbon into the bulk call occur at much lower temperatures. The reaction of carbon at high temperatures shows two regimes: (i) a non steady-state evolution of CO due to the clean-off of surface carbon already present on the surface, followed by (ii) a near steady-state reaction due to the continuous diffusion of carbon to the surface.
引用
收藏
页码:5060 / 5067
页数:8
相关论文
共 41 条
[1]   A SIMPLE MOLECULAR-BEAM SYSTEM FOR SURFACE REACTIVITY STUDIES [J].
BOWKER, M ;
PUDNEY, PDA ;
BARNES, CJ .
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A-VACUUM SURFACES AND FILMS, 1990, 8 (02) :816-820
[2]   Ethene adsorption, dehydrogenation and reaction with Pd(110): Pd as a carbon 'sponge' [J].
Bowker, M ;
Morgan, C ;
Perkins, N ;
Holroyd, R ;
Fourre, E ;
Grillo, F ;
MacDowall, A .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (06) :2377-2386
[3]   Acetic acid adsorption and decomposition on Pd(110) [J].
Bowker, M ;
Morgan, C ;
Couves, J .
SURFACE SCIENCE, 2004, 555 (1-3) :145-156
[4]   The molecular beam reactor [J].
Bowker, M .
APPLIED CATALYSIS A-GENERAL, 1997, 160 (01) :89-98
[5]  
BOWKER M, 2004, CATAL LETT, V98, P1
[6]   Acetaldehyde adsorption and catalytic decomposition on Pd(110) and the dissolution of carbon [J].
Bowker, Michael ;
Holroyd, Richard ;
Perkins, Nell ;
Bhantoo, Jenita ;
Counsell, Jonathan ;
Carley, Albert ;
Morgan, Chris .
SURFACE SCIENCE, 2007, 601 (17) :3651-3660
[7]   Structure and decomposition pathways of vinyl acetate on Pd(111) [J].
Calaza, F ;
Stacchiola, D ;
Neurock, M ;
Tysoe, WT .
SURFACE SCIENCE, 2005, 598 (1-3) :263-275
[8]  
CONRAD H, 1977, SURF SCI, V65, P245, DOI 10.1016/0039-6028(77)90305-3
[9]   APPLICATION OF ISOTOPIC TRANSIENT KINETICS TO VINYL-ACETATE CATALYSIS [J].
CRATHORNE, EA ;
MACGOWAN, D ;
MORRIS, SR ;
RAWLINSON, AP .
JOURNAL OF CATALYSIS, 1994, 149 (02) :254-267
[10]   The mechanism of palladium-catalyzed decomposition of ethanol - A comparison of chemical kinetic and surface science studies [J].
Davidson, JM ;
McGregor, CM ;
Doraiswamy, LK .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2001, 40 (01) :108-113