Materials Design of Core-Shell Nanostructure Catalysts and New Quantum Monte Carlo Methods, with Application to Combustion
Abstract
During the current grant period, we completed projects designed to understand the surface chemistry of polar oxides. We showed how oxide dipoles change bare and supported-metal chemistry, imparting charge to "'switchable nanocatalysts". We showed how changing gaseous conditions above oxides can change the bulk and surface structure, controlling surface chemistry. We also investigated how doping oxides changes their catalytic and light absorption properties. We demonstrated that metal cations can be incorporated accompanied by vacancies, leading to recycling of catalytic met- als as "intelligent catalysts". We showed that this effect enhances catalysis and improves visible light absorption for possible solar applications. We have developed new methods for improved modeling of surface chemical and light absorption properties. We showed the importance of going beyond the d-band center approximation to understand metal catalysis. and created new pseudopotentials to facilitate use of hybrid functionals for extended solids. Because oxides offer both visible light absorption and fruitful surface chemistry, some preliminary activities relating to water splitting reactivity have been undertaken toward the end of the grant period.
Document Details
- Document Type
- Technical Report
- Publication Date
- Feb 12, 2010
- Accession Number
- ADA589588
Entities
People
- Andrew M Rappe
Organizations
- University of Pennsylvania