Removal of elemental mercury with Mn/Mo/Ru/Al<sub>2</sub>O<sub>3</sub> membrane catalytic system

doi:10.1007/s11783-012-0430-y

Front Envir Sci Eng

0, Vol.

Issue () : 464-473 https://doi.org/10.1007/s11783-012-0430-y

RESEARCH ARTICLE

Removal of elemental mercury with Mn/Mo/Ru/Al₂O₃ membrane catalytic system

Yongfu GUO^1,2, Naiqiang YAN¹(

), Ping LIU¹, Shijian YANG¹, Juan WANG¹, Zan QU¹

1. School of Environmental Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China; 2. Department of Municipal Engineering, Suzhou University of Science and Technology, Suzhou 215011, China

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Abstract

In this work, a catalytic membrane using Mn/Mo/Ru/Al₂O₃ as the catalyst was employed to remove elemental mercury (Hg⁰) from flue gas at low temperature. Compared with traditional catalytic oxidation (TCO) mode, Mn/Al₂O₃ membrane catalytic system had much higher removal efficiency of Hg⁰. After the incorporation of Mo and Ru, the production of Cl₂ from the Deacon reaction and the retainability for oxidants over Mn/Al₂O₃ membrane were greatly enhanced. As a result, the oxidization of Hg⁰ over Mn/Al₂O₃ membrane was obviously promoted due to incorporation of Mo and Ru. In the presence of 8 ppmv HCl, the removal efficiency of Hg⁰ by Mn/Mo/Ru/Al₂O₃ membrane reached 95% at 423 K. The influence of NO and SO₂ on Hg⁰ removal were insignificant even if 200 ppmv NO and 1000 ppmv SO₂ were used. Moreover, compared with the TCO mode, the Mn/Mo/Ru/Al₂O₃ membrane catalytic system could remarkably reduce the demanded amount of oxidants for Hg⁰ removal. Therefore, the Mn/Mo/Ru/Al₂O₃ membrane catalytic system may be a promising technology for the control of Hg⁰ emission.

Keywords flue gas elemental mercury membrane catalysis transition metal

Corresponding Author(s): YAN Naiqiang,Email:nqyan@sjtu.edu.cn

Issue Date: 01 June 2013

Cite this article:

Yongfu GUO,Naiqiang YAN,Ping LIU, et al. Removal of elemental mercury with Mn/Mo/Ru/Al₂O₃ membrane catalytic system[J]. Front Envir Sci Eng, 0, (): 464-473.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-012-0430-y
https://academic.hep.com.cn/fese/EN/Y0/V/I/464

Fig.1 Experimental scheme of the MCs

Fig.2 X-ray diffraction patterns (a) Mn catalyst and (b) Mn-Mo-Ru catalyst

Tab.1 Composition and properties of different catalysts

Fig.3 Adsorption curves of Hg with catalysts doped with various transition metals, at 423 K, [HCl] = [SO] = 0, was about 24 ppbv, air was used as carrier gas except Mn/N with N as carrier gas

Fig.4 Removal efficiencies of Hg with the catalysts doped with various transition metals, at 423 K, [HCl] = 8 ppmv, [SO] = 0, was about 23.5 ppbv, and air was used as carrier gas

Fig.5 Influence of Cl on Hg removal with Mn-Mo-Ru catalyst, at 423 K, air as carrier gas, was about 23 ppbv, [Cl] = 0.5 ppmv, [SO] = [HCl] = 0

Fig.6 Influence on Hg removal with intermittent injection of HCl in the MCs and the TCO mode, [HCl] = 8 ppmv, was about 23 ppbv, air as carrier gas, [SO] = 0, Mn-Mo-Ru as catalyst, = 423 K

Fig.7 Influence of SO on the removal for Hg, was about 23 ppbv, air as carrier gas, = 423 K

Fig.8 Influence on Hg removal with various concentration of SO (a, [HCl] = [NO] = 0; b, [HCl] = 0, [NO] = 100 ppmv; c, [HCl] = 8 ppmv, [NO] = 0; d, [HCl] = 8 ppmv, [NO] = 100 ppmv; and e, [HCl] = 8 ppmv, [NO] = 200 ppmv. Air was used as carrier gas, Mn-Mo-Ru as catalyst, = 423 K, was about 23.2 ppbv)

Tab.2 Influence of NO on sulfur-tolerance with Mn-Mo-Ru catalyst and 8 ppmv HCl

Fig.9 TPR profiles and the peak results (a) Mn catalyst, (b) Mn-Mo-Ru catalyst (dash is fitted results), symbol denotes the area of corresponding reduction peak

Tab.3 Results of H2-TPR profiles of Mn and Mn-Mo-Ru catalysts

Fig.10 XPS spectroscopes of Mn 2p, Mo 3d, Ru 3d, Hg 4f and S 2P (dash is fitted results) (a) Mn 2p, N as carrier gas; (b) Mn 2p, air as carrier gas; (c) S 2p, air as carrier gas; (d) Mo 3d, air as carrier gas; (e) Ru 3d, air as carrier gas; (f) Hg 4f, air as carrier gas. Mn-Mo-Ru catalyst was used, was about 15-20 ppbv, [HCl] = 8 ppmv, [SO] = 1000 ppmv

Fig.11 Mercury speciation results of three replicate tests, Mn-Mo-Ru was used as catalyst, was about 23 ppbv, [HCl] = 8 ppmv, [SO] = 0, = 423 K

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