4.7 Article

Co-regulation of dispersion, exposure and defect sites on CeO2 (111) surface for catalytic oxidation of Hg0

Journal

JOURNAL OF HAZARDOUS MATERIALS
Volume 424, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.jhazmat.2021.126566

Keywords

Elemental mercury; Ce-based catalyst; Synergistic effect; DFT calculation; Mechanism

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CeO2-based catalysts show high efficiency in catalytic oxidation of Hg-0, with the synergistic interactions between Ce and Mo facilitating the formation of defect-containing surface sites. Regulating the dispersion, exposure, and defect sites on CeO2(111) surface provides a feasible approach to enhancing the oxidation of Hg-0 for efficient removal of environmental pollutants.
The additional cost of Hg-0 capture in coal-fired power plants has facilitated the demand for environmental pollutants mitigation material for Hg-0 oxidation to Hg2+ for an ultra-low Hg emission technology. Herein, a suite of CeO2-based catalysts were investigated aiming at ultra-low gaseous Hg-0 emission at coal-fired power stations. Gaseous elemental mercury is feasible to be catalytically oxidized to Hg2+. The co-regulated dispersion, exposure and defect sites on CeO2 (111) surface with 2 wt% Ce and 8 wt% Mo compositions on gamma-Al2O3 was found to be the most promising catalyst demonstrating a high catalytic oxidation efficiency, a broad operating temperature range and a low activation energy. Specifically, it is shown that the oxidation of Hg-0 on the Ce-based catalysts can be enhanced by the addition of Mo (up to 8 wt%) via promoting the CeO2 (111) surface dispersion and exposure. Moreover, insights into the Ce and Mo synergistic interactions showed that it facilitated the formation of defect-containing surface sites. Besides, the co-regulation of dispersion, exposure and defect sites on CeO2 (111) surface was further studied by DFT calculations. This study provides a feasible approach in optimization of CeO2-based catalysts for catalytic oxidation of Hg-0 to achieve efficient removal of environmental pollutants.

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