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2018, Volume 12, Issue 2

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Frontiers of Environmental Science & Engineering >> 2018, Volume 12, Issue 2 doi: 10.1007/s11783-018-1007-1

New insights into mercury removal mechanism on CeO

. Forestry College, Guizhou University, Guiyang 550025, China.. Key Laboratory of High-Temperature and High-Pressure Study of the Earth’s Interior, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550081, China.. State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, College of Energy, Beijing University of Chemical Engineering, Beijing 100029, China

Available online: 2017-11-07
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Abstract

First-principles calculations were performed to investigate the mechanism of Hg adsorption and oxidation on CeO (111). Surface oxygen activated by the reduction of Ce to Ce was vital to Hg adsorption and oxidation processes. Hg was fully oxidized by the surface lattice oxygen on CeO (111), without using any other oxidizing agents. HCl could dissociate and react with the Hg adatom on CeO (111) to form adsorbed Hg–Cl or Cl–Hg–Cl groups, which promoted the desorption of oxidized Hg and prevented CeO catalyst deactivation. In contrast, O–H and H–O–H groups formed during HCl adsorption consumed the active surface oxygen and prohibited Hg oxidation. The consumed surface oxygen was replenished by adding O into the flue gas. We proposed that oxidized Hg desorption and maintenance of sufficient active surface oxygen were the rate-determining steps of Hg removal on CeO -based catalysts. We believe that our thorough understanding and new insights into the mechanism of the Hg removal process will help provide guidelines for developing novel CeO -based catalysts and enhance the Hg removal efficiency.

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