Reaction of CH3OH on Pd/ZnO(0001) and PdZn/ZnO(0001) model catalysts

被引:35
作者
Bera, Parthasarathi [1 ]
Vohs, John M. [1 ]
机构
[1] Univ Penn, Dept Chem & Biomol Engn, Philadelphia, PA 19104 USA
关键词
D O I
10.1021/jp068501f
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 adsorption and reaction of CH3OH on Pd and PdZn films and particles supported on the (0001) surface of a ZnO single crystal were studied using temperature-programmed desorption (TPD). At 300 K, vapor-deposited Pd films followed a two-dimensional island growth mode and preferentially blocked the active sites for dissociative adsorption of methanol on the ZnO(0001) surface. Upon heating, the Pd films agglomerated into particles and reacted with the ZnO substrate to form a PdZn alloy. Methanol was found to undergo complete dehydrogenation on the supported Pd and PdZn films and particles producing CO and H-2. Consistent with previous studies, alloying of Pd with Zn decreased the strength of the interaction of CO with the metal surface, as evidenced by a decrease in the CO desorption temperature. A low-temperature pathway for the oxidation of CO to CO2 on Pd/ZnO(0001) and PdZn/ZnO(0001), in which oxygen was supplied by the ZnO(0001) support, was also identified.
引用
收藏
页码:7049 / 7057
页数:9
相关论文
共 52 条
[1]   Production of hydrogen from methanol over binary Cu/ZnO catalysts - Part II. Catalytic activity and reaction pathways [J].
Agrell, J ;
Boutonnet, M ;
Fierro, JLG .
APPLIED CATALYSIS A-GENERAL, 2003, 253 (01) :213-223
[2]   DECOMPOSITION OF METHANOL, FORMALDEHYDE, AND FORMIC-ACID ON NONPOLAR (101BARO), STEPPED (505BARI), AND (0001) SURFACES OF ZNO BY TEMPERATURE-PROGRAMMED DECOMPOSITION [J].
AKHTER, S ;
CHENG, WH ;
LUI, K ;
KUNG, HH .
JOURNAL OF CATALYSIS, 1984, 85 (02) :437-456
[3]   COMPARISON OF THE CHEMICAL-PROPERTIES OF THE ZINC-POLAR, THE OXYGEN-POLAR, AND THE NONPOLAR SURFACES OF ZNO [J].
AKHTER, S ;
LUI, K ;
KUNG, HH .
JOURNAL OF PHYSICAL CHEMISTRY, 1985, 89 (10) :1958-1964
[4]   Metal deposits on well-ordered oxide films [J].
Bäumer, M ;
Freund, HJ .
PROGRESS IN SURFACE SCIENCE, 1999, 61 (7-8) :127-198
[5]   Growth and structure of Pd films on ZnO(0001) [J].
Bera, Parthasarathi ;
Vohs, John M. .
JOURNAL OF CHEMICAL PHYSICS, 2006, 125 (16)
[6]   Studies of the water-gas-shift reaction on ceria-supported Pt, Pd, and Rh: implications for oxygen-storage properties [J].
Bunluesin, T ;
Gorte, RJ ;
Graham, GW .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 15 (1-2) :107-114
[7]   Ultrathin metal films and particles on oxide surfaces: Structural, electronic and chemisorptive properties [J].
Campbell, CT .
SURFACE SCIENCE REPORTS, 1997, 27 (1-3) :1-111
[8]   CU/ZNO(0001-BAR) AND ZNOX/CU(111) - MODEL CATALYSTS FOR METHANOL SYNTHESIS [J].
CAMPBELL, CT ;
DAUBE, KA ;
WHITE, JM .
SURFACE SCIENCE, 1987, 182 (03) :458-476
[9]   SPECTROSCOPIC STUDIES OF METHANOL DECOMPOSITION ON PD(111) [J].
CHEN, JJ ;
JIANG, ZC ;
ZHOU, Y ;
CHAKRABORTY, BR ;
WINOGRAD, N .
SURFACE SCIENCE, 1995, 328 (03) :248-262
[10]   Steam reforming of methanol over highly active Pd/ZnO catalyst [J].
Chin, YH ;
Dagle, R ;
Hu, JL ;
Dohnalkova, AC ;
Wang, Y .
CATALYSIS TODAY, 2002, 77 (1-2) :79-88