Hydrogen Dissociation, Spillover, and Desorption from Cu-Supported Co Nanoparticles

被引:39
作者
Lewis, Emily A. [1 ]
Marcinkowski, Matthew D. [1 ]
Murphy, Colin J. [1 ]
Liriano, Melissa L. [1 ]
Sykes, E. Charles H. [1 ]
机构
[1] Tufts Univ, Dept Chem, Medford, MA 02155 USA
关键词
CARBON-MONOXIDE; SURFACE SCIENCE; COBALT; ADSORPTION; MECHANISM; CATALYSTS; COPPER; CHEMISORPTION; PATHWAYS; KINETICS;
D O I
10.1021/jz5016789
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
Co-Cu nanoparticles have recently been explored for Fischer-Tropsch synthesis (FTS) as a way to combine the long chain selectivity of Co with Cu's activity for alcohol formation in order to synthesize oxygenated transportation fuels. Depending on particle size, hydrogen dissociation can be a rate-determining step in cobalt-catalyzed FTS. To understand the fundamentals of uptake and release of hydrogen from the Co/Cu bimetallic system, we prepared well-defined Co nanoparticles on Cu(111). We demonstrate that hydrogen spills over from dissociation sites on the Co nanoparticles to the Cu(111) surface via the Co-Cu interface and that desorption of H occurs at a temperature that is lower than from Co or Cu alone, which we attribute to the Co-Cu interface sites. From this data, we have constructed an energy landscape for the facile dissociation, spillover, and desorption of hydrogen on the Co-Cu bimetallic system.
引用
收藏
页码:3380 / 3385
页数:6
相关论文
共 44 条
[1]   Surface Composition Changes of Redox Stabilized Bimetallic CoCu Nanoparticles Supported on Silica under H2 and O2 Atmospheres and During Reaction between CO2 and H2: In Situ X-ray Spectroscopic Characterization [J].
Alayoglu, Selim ;
Beaumont, Simon K. ;
Melaet, Gerome ;
Lindeman, Avery E. ;
Musselwhite, Nathan ;
Brooks, Christopher J. ;
Marcus, Matthew A. ;
Guo, Jingua ;
Liu, Zhi ;
Kruse, Norbert ;
Somorjai, Gabor A. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2013, 117 (42) :21803-21809
[2]   ADSORPTION AND DESORPTION-KINETICS IN THE SYSTEMS H-2/CU(111), H-2/CU(110) AND H-2/CU(100) [J].
ANGER, G ;
WINKLER, A ;
RENDULIC, KD .
SURFACE SCIENCE, 1989, 220 (01) :1-17
[3]   An Atomic-Scale View of Palladium Alloys and their Ability to Dissociate Molecular Hydrogen [J].
Baber, Ashleigh E. ;
Tierney, Heather L. ;
Lawton, Timothy J. ;
Sykes, E. Charles H. .
CHEMCATCHEM, 2011, 3 (03) :607-614
[4]   Recent developments in the application of nanomaterials to understanding molecular level processes in cobalt catalysed Fischer-Tropsch synthesis [J].
Beaumont, S. K. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (11) :5034-5043
[5]   Exploring surface science and restructuring in reactive atmospheres of colloidally prepared bimetallic CuNi and CuCo nanoparticles on SiO2 in situ using ambient pressure X-ray photoelectron spectroscopy [J].
Beaumont, Simon K. ;
Alayoglu, Selim ;
Pushkarev, Vladimir V. ;
Liu, Zhi ;
Kruse, Norbert ;
Somorjai, Gabor A. .
FARADAY DISCUSSIONS, 2013, 162 :31-44
[6]   Single atom alloy surface analogs in Pd0.18Cu15 nanoparticles for selective hydrogenation reactions [J].
Boucher, Matthew B. ;
Zugic, Branko ;
Cladaras, George ;
Kammert, James ;
Marcinkowski, Matthew D. ;
Lawton, Timothy J. ;
Sykes, E. Charles H. ;
Flytzani-Stephanopoulos, Maria .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2013, 15 (29) :12187-12196
[7]   HYDROGEN CHEMISORPTION AND THE CARBON MONOXIDE HYDROGEN INTERACTION ON COBALT(0001) [J].
BRIDGE, ME ;
COMRIE, CM ;
LAMBERT, RM .
JOURNAL OF CATALYSIS, 1979, 58 (01) :28-33
[8]   Dealloying of Cobalt from CuCo Nanoparticles under Syngas Exposure [J].
Carenco, Sophie ;
Tuxen, Anders ;
Chintapalli, Mahati ;
Pach, Elzbieta ;
Escudero, Carlos ;
Ewers, Trevor D. ;
Jiang, Peng ;
Borondics, Ferenc ;
Thornton, Geoff ;
Alivisatos, A. Paul ;
Bluhm, Hendrik ;
Guo, Jinghua ;
Salmeron, Miguel .
JOURNAL OF PHYSICAL CHEMISTRY C, 2013, 117 (12) :6259-6266
[9]   SCANNING-TUNNELING-MICROSCOPY STUDY OF THE GROWTH OF COBALT ON CU(111) [J].
DELAFIGUERA, J ;
PRIETO, JE ;
OCAL, C ;
MIRANDA, R .
PHYSICAL REVIEW B, 1993, 47 (19) :13043-13046
[10]   Mechanism and kinetics of the catalytic CO-H2 reaction:: An approach by chemical transients and surface relaxation spectroscopy [J].
Frennet, A ;
de Bocarmé, TV ;
Bastin, JM ;
Kruse, N .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (06) :2350-2359