(335a) Applications of the Reaxff Method to Metal and Metal Oxide Surface Chemistry

The ReaxFF method provides a highly transferable simulation method for atomistic scale simulations on chemical reactions at the nanosecond and nanometer scale. It combines concepts of bond-order based potentials with a polarizable charge distribution.

Since it initial development for hydrocarbons in 2001 [1], we have found this concept to be highly transferable, leading to applications to elements all across the periodic table, including all first row elements, metals, ceramics and ionic materials (for example, [2-5]). For all these elements and associated materials we have demonstrated that ReaxFF can accurately reproduce quantum mechanics (QM)-based structures, reaction energies and reaction barriers, enabling the method to predict reaction kinetics in complicated, multi-material environments at a relatively modest computational expense.

In this presentation we will provide an overview of recent developments of the ReaxFF method, including its availability in parallel simulation environments, and recent application of this method to simulations on reactions at metal and metal oxide interfaces. In particular, we will discuss recent results of ReaxFF simulations on water/TiO₂ interfaces [6], protein/TiO₂ interfaces [7] and hydrocarbon catalytic conversion reactions at iron [8] and palladium surfaces. In all these cases we will describe how the ReaxFF parameters were developed by training against a predominantly QM based data set and how these parameters were subsequently used to perform a series of simulations that could be directly or indirectly validated against experiment. 

[1] van Duin, A. C. T.; Dasgupta, S.; Lorant, F.; Goddard, W. A. Journal of Physical Chemistry A 2001, 105, 9396.

[2] Weismiller, M. R.; van Duin, A. C. T.; Lee, J.; Yetter, R. A. J. Phys. Chem. A  2010, 114, 5485.

[3] van Duin, A. C. T.; Bryantsev, V. S.; Diallo, M. S.; Goddard, W. A.; Rahaman, O.; Doren, D. J.; Raymand, D.; Hermansson, K. Journal of Physical Chemistry A 2010, 114, 9507.

[4] Joshi, K.; van Duin, A. C. T.; Jacob, T. Journal of Materials Chemistry 2010, 20, 10431.

[5] Fogarty, J. C.; Aktulga, H. M.; Grama, A. Y.; van Duin, A. C. T.; Pandit, S. A. J. Chem. Phys. 2010, 132, 174704/1.

[6] Kim, S.-Y.; Kumar, N.; Persson, P.; Sofo, J.; van Duin, A. C. T.; Kubicki, J. D. J. Comp. Chem. 2012, submitted.

[7] Monti, S.; van Duin, A. C. T.; Kim, S.-Y.; Barone, V. J.Phys.Chem. A  2012, 116, 5141.

[8] Zou, C.; van Duin, A. C. T.; Sorescu, D. Topics in Catalysis 2012, in print.