Research on the Mechanism of Elemental Mercury Removal over Mn-Based SCR Catalysts by a Developed Hg-TPD Method

汞元素 催化作用 Mercury(编程语言) 化学 选择性催化还原 无机化学 环境化学 核化学 吸附 物理化学 有机化学 计算机科学 程序设计语言
作者
Shibo Zhang,Mercedes Dı́az-Somoano,Yongchun Zhao,Jianping Yang,Junying Zhang
出处
期刊:Energy & Fuels [American Chemical Society]
卷期号:33 (3): 2467-2476 被引量:42
标识
DOI:10.1021/acs.energyfuels.8b04424
摘要

Using an selective catalytic reduction (SCR) catalyst to oxidize and remove elemental mercury (Hg 0 ) synergistically is a promising method for mercury emission control in coal combustion power plants and is currently attracting widespread interest. In this study, a developed mercury thermal desorption (Hg-TPD) approach, combined with other associated methods, was employed for the identification of mercury species in the Mn-based SCR catalysts that have been used for synergistic Hg 0 removal. The analysis results demonstrated that the Hg 0 adsorption on the catalysts was a necessary process for the Hg 0 removal, though the SCR catalysts removed Hg 0 mainly through catalytic oxidation and the amount of the adsorbed mercury contributed only a little to the Hg 0 removal efficiency. This essential adsorption process was mainly realized through chemisorption. HgO was the prime species that was identified to form in the catalysts, and a little amount of adsorbed HgCl 2, Hg(NO 3 ) 2, and Hg-OM was detected as well in the samples spent in the simulated coal-fired flue gases. O 2, HCl, NO, and high concentration of CO 2 in the flue gas all promoted the adsorption capacity and the generation of the related Hg compounds, so that they were conductive to Hg 0 removal efficiency, whereas a similar phenomenon was not observed in the presence of SO 2, NH 3, and H 2 O, and meanwhile the amount of adsorbed HgO was decreased, so that the efficiency was inhibited. The mobility testing by a sequential extraction procedure indicated that most of the retained Hg belonged to the mobile fraction, which was in accordance with the identification results of the Hg-TPD analysis. The consequences of this research would create a better understanding of the Hg 0 removal mechanism over the Mn-based SCR catalysts and provide additional information on the disposal of the retired catalysts in the environment.

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