Rhodium Catalysts in the Oxidation of CO by O2 and NO: Shape, Composition, and Hot Electron Generation
- Univ. of California, Berkeley, CA (United States)
It is well known that the activity, selectivity, and deactivation behavior of heterogeneous catalysts are strongly affected by a wide variety of parameters, including but not limited to nanoparticle size, shape, composition, support, pretreatment conditions, oxidation state, and electronic state. Enormous effort has been expended in an attempt to understand the role of these factors on catalytic behavior, but much still remains to be discovered. In this work, we have focused on deepening the present understanding of the role of nanoparticle shape, nanoparticle composition, and hot electrons on heterogeneous catalysis in the oxidation of carbon monoxide by molecular oxygen and nitric oxide. These reactions were chosen because they are important for environmental applications, such as in the catalytic converter, and because there is a wide range of experimental and theoretical insight from previous single crystal work as well as experimental data on nanoparticles obtained using new state-of-the-art techniques that aid greatly in the interpretation of results on complex nanoparticle systems. In particular, the studies presented in this work involve three types of samples: ~ 6.5 nm Rh nanoparticles of different shapes, ~ 15 nm Rh1-xPdx core-shell bimetallic polyhedra nanoparticles, and Rh ultra-thin film (~ 5 nm) catalytic nanodiodes. The colloidal nanoparticle samples were synthesized using a co-reduction of metal salts in alcohol and supported on silicon wafers using the Langmuir-Blodgett technique. This synthetic strategy enables tremendous control of nanoparticle size, shape, and composition. Nanoparticle shape was controlled through the use of different organic polymer capping layers. Bimetallic core-shell nanoparticles were synthesized by careful choice of metal salt precursors. Rh/TiOx and Rh/GaN catalytic nanodiodes were fabricated using a variety of thin film device fabrication techniques, including reactive DC magnetron sputtering, electron beam evaporation, and rapid thermal annealing. The combination of these techniques enabled control of catalytic nanodiode morphology, geometry, and electrical properties.
- Research Organization:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- DOE Contract Number:
- AC02-05CH11231
- OSTI ID:
- 983012
- Report Number(s):
- LBNL-3167E; TRN: US201014%%769
- Resource Relation:
- Related Information: Designation of Academic Dissertation: Doctoral; Academic Degree: Ph.D.; Name of Academic Institution: UC Berkeley
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
CARBON MONOXIDE
CATALYSTS
CATALYTIC CONVERTERS
DEACTIVATION
ELECTRICAL PROPERTIES
ELECTRON BEAMS
ELECTRONS
EVAPORATION
FABRICATION
HETEROGENEOUS CATALYSIS
MAGNETRONS
MONOCRYSTALS
MORPHOLOGY
NITRIC OXIDE
ORGANIC POLYMERS
OXIDATION
RHODIUM
SILICON
THIN FILMS
VALENCE