期刊
MATERIALS
卷 11, 期 4, 页码 -出版社
MDPI
DOI: 10.3390/ma11040485
关键词
Hg-0 oxidation mechanism; surface oxygen; CeO2 (111) surface; DFT study
类别
资金
- National Basic Research Program of China [2015CB251501]
- National Natural Science Foundation of China [51576064]
- Beijing Nova Program [Z171100001117064]
- Beijing Natural Science Foundation [3172030]
- Fok Ying Tung Education Foundation [161051]
- Fundamental Research Funds for the Central Universities [2018ZD08, 2016YQ05]
CeO2 is a promising catalytic oxidation material for flue gas mercury removal. Density functional theory (DFT) calculations and periodic slab models are employed to investigate mercury adsorption and oxidation by oxygen over the CeO2 (111) surface. DFT calculations indicate that Hg-0 is physically adsorbed on the CeO2 (111) surface and the Hg atom interacts strongly with the surface Ce atom according to the partial density of states (PDOS) analysis, whereas, HgO is adsorbed on the CeO2 (111) surface in a chemisorption manner, with its adsorption energy in the range of 69.9-198.37 kJ/mol. Depending on the adsorption methods of Hg-0 and HgO, three reaction pathways (pathways I, II, and III) of Hg-0 oxidation by oxygen are proposed. Pathway I is the most likely oxidation route on the CeO2 (111) surface due to it having the lowest energy barrier of 20.7 kJ/mol. The formation of the HgO molecule is the rate-determining step, which is also the only energy barrier of the entire process. Compared with energy barriers of Hg-0 oxidation on the other catalytic materials, CeO2 is more efficient at mercury removal in flue gas owing to its low energy barrier.
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