期刊
FUEL
卷 327, 期 -, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.fuel.2022.125200
关键词
Hg 0 removal; Syngas; Fe7SC sorbent; Removal mechanism; Density functional theory
资金
- National Natural Science Foundation of China [51976108, U1906232]
- Key R & D Project of Shandong Province, China [2020CXGC011402]
- Natural Science Foundation of Xinjiang Uygur Autonomous Region [2022D01C07]
- Zhejiang Provincial Department of Science and Technology [2020E10018]
In this study, a Fe7SC sorbent was prepared for the removal of Hg0 from simulated syngas by introducing oxygen to induce H2S oxidation for enhanced capture of Hg0. Fe7SC demonstrated superior Hg0 removal performance in the presence of H2S + O2. CO and H2 suppressed Hg0 adsorption, while H2O inhibited Hg0 removal due to competitive adsorption.
In this study, a Fe7SC sorbent was prepared via hydrothermal impregnation and used to eliminate Hg0 from simulated syngas. A certain amount of oxygen was introduced to induce targeted H2S oxidation to form active surface sulfur species for the enhanced capture of Hg0 over Fe7SC. The effects of the introduced oxygen, temperature, and syngas composition (H2S, CO, H-2, and H2O) on Hg0 adsorption performance were investigated. X-ray photoelectron spectroscopy, Hg-0-temperature programmed desorption, and density functional theory calculations were performed to elucidate the Hg-0 removal mechanism. Fe7SC exhibited a superior Hg-0 removal performance (approximately 99.2%) in the presence of H2S + O-2 at 150 ?C. The interaction between H2S and the introduced oxygen was responsible for its superior Hg-0 capture capacity. CO and H-2 suppressed Hg0 adsorption, and H2O inhibited Hg-0 removal owing to competitive adsorption. Results of the Bangham kinetic analysis indicate that Hg-0 surface chemisorption is the primary rate-controlling step. Hg0 adsorption on the Fe7SC sorbent may follow the Eley-Rideal mechanism, in which the active sulfur species generated from H2S oxidation react with gaseous Hg0 to form HgS.
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