Removal of elemental mercury from flue gas by Fe/Al-SiO<sub>2</sub> complex

LI Yang; CHEN Wei; ZHAO Yong-chun; LI Hai-long; ZHANG Jun-ying; LI Jie; HU Hao-quan

Volume 47 Issue 12

Dec. 2019

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Article Navigation > Journal of Fuel Chemistry and Technology > 2019 > 47(12): 1409-1416

LI Yang, CHEN Wei, ZHAO Yong-chun, LI Hai-long, ZHANG Jun-ying, LI Jie, HU Hao-quan. Removal of elemental mercury from flue gas by Fe/Al-SiO2 complex[J]. Journal of Fuel Chemistry and Technology, 2019, 47(12): 1409-1416.

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LI Yang, CHEN Wei, ZHAO Yong-chun, LI Hai-long, ZHANG Jun-ying, LI Jie, HU Hao-quan. Removal of elemental mercury from flue gas by Fe/Al-SiO₂ complex[J]. Journal of Fuel Chemistry and Technology, 2019, 47(12): 1409-1416.

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Removal of elemental mercury from flue gas by Fe/Al-SiO₂ complex

1.
State Key Laboratory of Fine Chemicals, Institute of Coal Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
2.
State Key of Coal Combustion, Huazhong University of Science and Technology, Wuhan 430074, China
3.
School of Energy Science and Engineering, Central South University, Changsha 410083, China
4.
School of Environmental Science and Technology, Dalian 116024, China

Funds:

the National Natural Science Foundation of China 21776039

National Natural Science Foundation for Young Scientist of China 51306028

the Fundamental Research Funds for the Central Universities DUT2018TB0

More Information

Corresponding author: HU Hao-quan, Tel: 0411-84986157, E-mail: hhu@dlut.edu.cn
Received Date: 2019-05-14
Rev Recd Date: 2019-10-17

Available Online: 2021-01-23

Publish Date: 2019-12-10

Abstract

Abstract

The Fe/Al-SiO₂ composite metal oxides were prepared by various methods to simulate the composition of red mud. A series of experiments were carried out to study the mercury removal performance from simulated flue gas. The results show that the composite metal oxide obtained by sol-gel method has an excellent mercury removal performance in a temperature range of 300-450 ℃. Among them, average mercury removal efficiency can reach 94.8% within 3 h at 350 ℃. Fe₂O₃ provides lattice oxygen and chemical adsorbed oxygen for the oxidation of Hg⁰, and SiO₂ is conducive to the dispersion of the active component Fe₂O₃, which enhances the contact between Hg⁰ and the active sites. In the presence of trace HCl and NO in flue gas, the removal efficiency of Hg⁰ is close to 100%. However, the average mercury removal efficiency reduces to 90.7% and 53.4% respectively after adding 0.2 mL/min and 0.4 mL/min SO₂, since the reaction of SO₂ and Fe₂O₃ produces Fe₂(SO₄)₃, leading to the deactivation of Fe₂O₃.
- sorbents,
- elemental mercury,
- flue gas,
- Fe/Al-SiO₂

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References(30)

References

[1]	UNEP. Global Mercury Assessment 2018 Review Draft: Sources, Emissions, Releases and Environmental Transport. Geneva: UNEP Chemicals Branch. 2018.
[2]	DB14/T1703, 燃煤电厂大气污染物排放标准[S]. DB14/T1703, Standard emissions of atmospheric pollutants for coal-fired power plants[S].
[3]	YANG J, YANG Q, SUN J, LIU Q C, ZHAO D, GAO W, LIU L. Effects of mercury oxidation on V₂O₅-WO₃/TiO₂ catalyst properties in NH₃-SCR process[J]. Catal Commun, 2015, 59:78-82. doi: 10.1016/j.catcom.2014.09.049
[4]	HSU C J, CHIOU H J, CHEN Y H, LIN K S, ROOD M J, HIS H C. Mercury adsorption and re-emission inhibition from actual WFGD wastewater using sulfur-containing activated carbon[J]. Environ Res, 2019, 168:319-328. doi: 10.1016/j.envres.2018.10.017
[5]	GRANITE E J, PENNLINE H W, HARGIS R A. Novel sorbents for mercury removal from flue gas[J]. Ind Eng Chem Res, 2000, 39(4):1020-1029. doi: 10.1021/ie990758v
[6]	ZHAO S L, PUDASAINEE D, DUAN Y F, GUPTA R, LIU M. A review on mercury in coal combustion process:Content and occurrence forms in coal, transformation, sampling methods, emission and control technologies[J]. Prog Energy Combust, 2019, 73:26-64. doi: 10.1016/j.pecs.2019.02.001
[7]	WANG P Y, SU S, XIANG J, CAO F, SUN L S, HU S, LEI S Y. Catalytic oxidation of Hg⁰ by CuO-MnO₂-Fe₂O₃/γ-Al₂O₃ catalyst[J]. Chem Eng J, 2013, 225:68-75. doi: 10.1016/j.cej.2013.03.060
[8]	郝凯辉.改性赤泥基吸附剂用于燃煤烟气中汞的脱除[D].大连: 大连理工大学, 2017. http://cdmd.cnki.com.cn/Article/CDMD-10141-1017823742.htm HAO Kai-hui. Removal of elemental mercury from flue gas over modified red mud based sorbents[D]. Dalian: Dalian University of Technology, 2017. http://cdmd.cnki.com.cn/Article/CDMD-10141-1017823742.htm
[9]	CAO S T, MA H J, ZHANG Y, CHEN X F, ZHANG Y F. The phase transition in Bayer red mud from China in high caustic sodium aluminate solutions[J]. Hydrometallurgy, 2013, 140:111-119. doi: 10.1016/j.hydromet.2013.09.009
[10]	KHAIRUL M A, ZANGANEH J, MOGHTADERI B. The composition, recycling and utilisation of Bayer red mud[J]. Resour Conserv Recycl, 2019, 141:483-498. doi: 10.1016/j.resconrec.2018.11.006
[11]	WANG X P, SUN T C, WU S C, CHEN C, KOU J, XU C Y. A novel utilization of Bayer red mud through co-reduction with a limonitic laterite ore to prepare ferronickel[J]. J Cleaner Prod, 2019, 216:33-41. doi: 10.1016/j.jclepro.2019.01.176
[12]	SKODRAS G, DIAMANTOPOULOU I, SAKELLAROPOULOS G P. Role of activated carbon structural properties and surface chemistry in mercury adsorption[J]. Desalination, 2007, 210(1/3):281-286. http://cn.bing.com/academic/profile?id=f781b1d179ff7b246f08f94ee79af493&encoded=0&v=paper_preview&mkt=zh-cn
[13]	KONG F H, QIU J R, LIU H, ZHAO R, AI Z H. Catalytic oxidation of gas-phase elemental mercury by nano-Fe₂O₃[J]. J Environ Sci (China), 2011, 23(4):699-704. doi: 10.1016/S1001-0742(10)60438-X
[14]	ZHANG A C, ZHANG Z H, SHI J M, CHEN G Y, ZHOU C S, SUN L S. Effect of preparation methods on the performance of MnO_x-TiO₂ adsorbents for Hg⁰ removal and SO₂ resistance[J]. J Fuel Chem Technol, 2015, 43(10):1258-1266. doi: 10.1016/S1872-5813(15)30038-4
[15]	LIAO Y, XIONG S C, DANG H, XIAO X, YANG S J, WONG P K.The centralized control of elemental mercury emission from the flue gas by a magnetic rengenerable Fe-Ti-Mn spinel[J]. J Hazard Mater, 2015, 299:740-746. doi: 10.1016/j.jhazmat.2015.07.083
[16]	LIU T, MAN C Y, GUO X, ZHENG C G. Experimental study on the mechanism of mercury removal with Fe₂O₃ in the presence of halogens:Role of HCl and HBr[J]. Fuel, 2016, 173:209-216. doi: 10.1016/j.fuel.2016.01.054
[17]	KO K B, BYAN Y C, CHO M Y, NAMKUNG W, SHIN D N, KOH D J, KIM K T. Influence of HCl on oxidation of gaseous elemental mercury by dielectric barrier discharge process[J]. Chemosphere, 2008, 71(9):1674-1682. doi: 10.1016/j.chemosphere.2008.01.015
[18]	ZHANG A C, ZHENG W W, SONG J, HU S, LIU Z C, XIANG J. Cobalt manganese oxides modified titania catalysts for oxidation of elemental mercury at low flue gas temperature[J]. Chem Eng J, 2014, 236:29-38. doi: 10.1016/j.cej.2013.09.060
[19]	LIU W, XU H M, LIAO Y, QUAN Z W, LI S C, ZHAO S J, QU Z, YAN N Q. Recyclable CuS sorbent with large mercury adsorption capacity in the presence of SO₂ from non-ferrous metal smelting flue gas[J]. Fuel, 2019, 235:847-854. doi: 10.1016/j.fuel.2018.08.062
[20]	GUEDES A, VALENTIM B, PRIETO A C, SANZ A, FLORES D, NORONHA F. Characterization of fly ash from a power plant and surroundings by micro-Raman spectroscopy[J]. Int J Coal Geol, 2008, 73(3/4):359-370. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=839549dab048935e88e06e3379ac5366
[21]	DONG Y, REN X Y, QU R Y, LIU S J, ZHENG C H, GAO X. Designing SO₂-resistant cerium-based catalyst by modifying with Fe₂O₃ for the selective catalytic reduction of NO with NH₃[J]. Mol Catal, 2019, 462:10-18. doi: 10.1016/j.mcat.2018.10.007
[22]	XIANG J, WANG P Y, SU S, ZHANG L Q, CAO F, SUN Z J, XIAO X, SUN L S, H U S. Control of NO and Hg⁰ emissions by SCR catalysts from coal-fired boiler[J]. Fuel Process Technol, 2015, 135:168-173. doi: 10.1016/j.fuproc.2014.12.044
[23]	LIU J, GUO R T, GUAN Z Z, SUN X, PAN W G, LIU X Y, WANG Z Y, SHI X, QIN H, QIU Z Z, LIU S W. Simultaneous removal of NO and Hg⁰ over Nb-modified MnTiO_x catalyst[J]. Int J Hydrogen Energy, 2019, 44(2):835-843. doi: 10.1016/j.ijhydene.2018.11.006
[24]	KIM S C, NAHM S W, PARK Y K. Property and performance of red mud-based catalysts for the complete oxidation of volatile organic compounds[J]. J Hazard Mater, 2015, 300:104-113. doi: 10.1016/j.jhazmat.2015.06.059
[25]	HE C, SHEN B X, LI F K. Effects of flue gas components on removal of elemental mercury over Ce-MnO_x/Ti-PILCs[J]. J Hazard Mater, 2016, 304:10-17. doi: 10.1016/j.jhazmat.2015.10.044
[26]	LI G L, SHEN B X, LI Y W, ZHAO B, WANG F M, HE C, WANG Y Y, ZHANG M. Removal of element mercury by medicine residue derived biochars in presence of various gas compositions[J]. J Hazard Mater, 2015, 298:162-169. doi: 10.1016/j.jhazmat.2015.05.031
[27]	CHEN Y, GUO X, WU F, HUANG Y, YIN Z C. Mechanisms of mercury transformation over α-Fe₂O₃ (001) in the presence of HCl and/or H₂S[J]. Fuel, 2018, 233:309-316. doi: 10.1016/j.fuel.2018.06.065
[28]	JIANG S J, LIU X, LI H L, WANG J, YANG Z Q, PENG H Y, SHI K M. Synergistic effect of HCl and NO in elemental mercury catalytic oxidation over La₂O₃-TiO₂ catalyst[J]. Fuel, 2018, 215:232-238 doi: 10.1016/j.fuel.2017.11.015
[29]	ZHENG J M, SHAH K J, ZHOU J S, PAN S Y, CHIANG P C. Impact of HCl and O₂ on removal of elemental mercury by heat-treated activated carbon:Integrated X-ray analysis[J]. Fuel Process Technol, 2017, 167:11-17. doi: 10.1016/j.fuproc.2017.06.017
[30]	YANG Y J, LIU J, WANG Z, LIU F. Heterogeneous reaction kinetics of mercury oxidation by HCl over Fe₂O₃ surface[J]. Fuel Process Technol, 2017, 159:266-271. doi: 10.1016/j.fuproc.2017.01.035