Dynamic Simulation of the Thermal Decomposition of Pyrite Under Vacuum

Abstract

The ultrasoft pseudopotential plane wave method is applied to dynamic simulation of the thermal decomposition mechanism of FeS2 under vacuum. The FeS2 (100), (111), and (210) surface relaxation and the geometric and electronic structure of the reactants and products are calculated. The results indicate that FeS2 (100) is the most preferred surface to dissociate and also the most common cleavage surface. The thermal decomposition mechanism of FeS2 is explained by dynamic simulation on a micro stratum: in general, the S-Fe bond gradually elongated until it fractured, the S-S bond strengthened gradually, the S-Fe bond was cleaved to form S, the force is relatively weaker between different layers, and thermal decomposition occurred easily between the layers. Simultaneously, the intermediate products, such as FexSy, were formed. Evidence of Fe pyrolysis into Fe metal was not found, and the intermediate products decomposed further. The contributions of the p and d orbitals of Fe increased, whereas that of the s orbital decreased. The contributions of the s and p orbitals of S decreased. The results obtained from FeS2 thermal decomposition experiments under vacuum and differential thermal analysis—thermogravimetry are consistent with the results of calculation and simulation.