Chemical reactions of oily sludge catalyzed by iron oxide under supercritical water gasification condition

Abstract

Supercritical water gasification is a promising technology in dealing with the degradation of hazardous waste, such as oily sludge, accompanied by the production of fuel gases. To evaluate the mechanism of Fe₂O₃ catalyst and the migration pathways of heteroatoms and to investigate the systems during the process, reactive force field molecular dynamics simulations are adopted. In terms of the catalytic mechanisms of Fe₂O₃, the surface lattice oxygen is consumed by small carbon fragments to produce CO and CO₂, improving the catalytic performance of the cluster due to more unsaturated coordination Fe sites exposed. Lattice oxygen combines with •H radicals to form water molecules, improving the catalytic performance. Furthermore, the pathway of asphaltene degradation was revealed at an atomic level, as well as products. Moreover, the adsorption of hydroxyl radical on the S atom caused breakage of the two C–S bonds in turn, forming •HSO intermediate, so that the organic S element was fixed into the inorganic liquid phase. The heteroatom O was removed under the effects of supercritical water. Heavy metal particles presented in the oily sludge, such as iron in association with Fe₂O₃ catalyst, helped accelerate the degradation of asphaltenes.

Graphical abstract

Keywords

oily sludge / SCWG / ReaxFF / Fe₂O₃ / heteroatoms

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Acknowledgments

This work was supported by the National Natural Science Foundation of China (Grant Nos. 21978210 and U20A20151), Tianjin Natural Science Foundation, China (Grant No. 19JCYBJC20000) and the National Key R&D Program of China (Grant No. 2018YFA0702403). The Gaussian 09 software was supported by the National Supercomputing Center in Shenzhen.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://dx.doi.org/10.1007/s11705-021-2125-z and is accessible for authorized users.

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