Quantum Chemistry
The group's work on population balance modelling has allowed particle interactions to be coupled with detailed gas-phase and surface chemistry mechanisms enabling very detailed modelling of nanoparticle synthesis processes. For many systems however, the detailed chemistry mechanisms required for this modelling are currently unknown. Recent advances in computational chemistry and computer power allow the necessary thermochemical information and activation energies to be calculated ab initio.
The gas phase oxidation of TiCl4 to form titanium dioxide (TiO2) nanoparticles has been performed in industry for over 50 years, and is the main production method for millions of tonnes of titania pigment each year. Despite the importance of this process, the detailed chemistry remains unknown.
To make progress with this project, we are using Density Functional Theory (DFT) to determine the thermochemistry of intermediate species and transition states for the chemical mechanism. We are also using Plane-Wave DFT to investigate adsorption, diffusion, and reaction of species on the surface of a TiO2 crystal, essential for detailed understanding of the surface-growth mechanisms of these nanoparticles.
The picture shows the highest occupied molecular orbital of the species Ti2O2Cl4, an intermediate in the oxidation of TiCl4.
Recent Associated Preprints
117: The Semantics of Chemical Markup Language (CML) for Computational Chemistry: CompChem
ref: Technical Report 117, c4e-Preprint Series, Cambridge, 2012 by Weerapong Phadungsukanan, Markus Kraft, Joe Townsend, and Peter Murray-Rust
100: Theoretical insights into the surface growth of rutile TiO2
ref: Technical Report 100, c4e-Preprint Series, Cambridge, 2011 by Raphael Shirley, Jethro Akroyd, Luke Miller, Oliver R. Inderwildi, Uwe Riedel, and Markus Kraft
97: First-principles thermochemistry for gas phase species in an industrial rutile chlorinator
ref: Technical Report 97, c4e-Preprint Series, Cambridge, 2010 by Raphael Shirley, Weerapong Phadungsukanan, Markus Kraft, Jim Downing, Nick Day, and Peter Murray-Rust
Recent Associated Publications
The semantics of Chemical Markup Language (CML) for computational chemistry: CompChem,
Weerapong Phadungsukanan, Markus Kraft, Joe Townsend, and Peter Murray-Rust, Journal of Cheminformatics , 4, 15, (2012)
A quantitative study of the clustering of polycyclic aromatic hydrocarbons at high temperatures,
Tim Totton, Alston Misquitta, and Markus Kraft, Physical Chemistry Chemical Physics , 14, 4081-4096, (2012)
A survey of the potential energy surface for the (benzene)13 cluster,
Dwaipayan Chakrabarti, Tim Totton, Markus Kraft, and David Wales, Physical Chemistry Chemical Physics , 13, 21362–21366, (2011)
Recent Associated Presentations
- Invited presentation by Markus Kraft Download: PDF (30.49 MB)
- Invited presentation by Markus Kraft
- Self Assembly Workshop Cambridge, 22nd September, 2011
- Invited presentation by Tim Totton Download: PDF (1.9 MB)
- Invited presentation by Tim Totton
Funding
Funding has generously been provided by Huntsman.