Influence of ZnCl2 solution impregnation on the surface properties of lignite semi-coke and its mercury removal performance at elevated temperature
WANG Li, CHEN Jiang-yan, ZHAO Ke, ZHANG Hua-wei
State Key Laboratory of Mining Disaster Prevention and Control Co-founded by Shandong Province and the Ministry of Science and Technology, Shandong University of Science and Technology, Qingdao 266590, China
The modified semi-coke (ZSC) was obtained by the pyrolysis of ZnCl2-impregnated lignite at 700℃. N2 adsorption/desorption, Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy were used to characterize the surface physical and chemical properties of original and modified semi-coke, and the gaseous elemental mercury (Hg0) removal performance of two kinds of semi-coke has been investigated in a lab-scale fixed-bed reactor. The experimental results showed that ZSC had more developed hole structure, large specific surface area and abundant C—Cl groups. The mercury removal efficiency of ZSC decreased as the adsorption temperature was raised in the temperature range of 100℃ to 360℃. Generally, the ZSC exhibited good mercury removal performance at elevated temperatures. During the chemisorption process, the Hg0 was partly oxidized to HgCl or HgCl2 by C—Cl groups, and the others reacted with oxygen contained functional groups on the surface of semi-coke to generate HgO simultaneously. Finally, the Hg0 was captured in the form of HgCl2 or HgO on the surface of semi-coke.
王力, 陈江艳, 赵可, 张华伟. ZnCl2溶液对褐煤半焦表面性质及其中高温脱汞性能的影响[J]. 中国环境科学, 2016, 36(3): 702-708.
WANG Li, CHEN Jiang-yan, ZHAO Ke, ZHANG Hua-wei. Influence of ZnCl2 solution impregnation on the surface properties of lignite semi-coke and its mercury removal performance at elevated temperature. CHINA ENVIRONMENTAL SCIENCECE, 2016, 36(3): 702-708.
Zhou Z J, Liu X W, Zhao B, et al. Effects of existing energy saving and air pollution control devices on mercury removal in coal-fired power plants[J]. Fuel Processing Technology, 2015, 131:99-108.
[2]
Kamata H, Ueno S, Sato N, et al. Mercury oxidation by hydrochloric acid over TiO2 supported metal catalysts in coal combustion flue gas[J]. Fuel Processing Technology, 2009, 90(7/8):947-951.
Presto A A, Granite E J. Noble metal catalysts for mercury oxidation in utility flue gas[J]. Platinum metals review, 2008, 52(3):144-154.
[6]
Li Y, Zhang J Y, Zhao Y C, et al. Volatility and speciation of mercury during pyrolysis and gasification of five Chinese coals[J]. Energy and Fuels, 2011,25(9):3988-3996.
Hsi H C, Tsai C Y, Lin K J. Impact of surface functional groups, water vapor, and flue gas components on mercury adsorption and oxidation by sulfur-impregnated activated carbons[J]. Energy and Fuels, 2014,28:3300-3309.
Tao S S, Li C T, Fan X P, et al. Activated coke impregnated with cerium chloride used for elemental mercury removal from simulated flue gas[J]. Chemical Engineering Journal, 2012,210: 547-556.
Zhang H W, Liu S S, Chen J T, et al. Research on the preparation of silver-loaded semi-coke and its adsorption characteristics to gas-phase Hg0 [J]. Advanced Materials Research, 2012,356-360: 1350-1355.
[17]
Zhang H W, Liu X L, Wang L, et al. Effects of acid treatments on surface property and mercury removal performance of lignite semi-coke[J]. Asian Journal of Chemistry, 2014,26(13):1-6.
Biniak S, Siedlewski J, Swiatkowski A, et al. The characterization of activated carbons with oxygen and nitrogen surface groups[J]. Carbon, 1997,35(12):1799-1810.
Philippc B, Peggy F, Denise C, et al. The characterization of nitrogen-enriched activated carbons by IR, XPS and LSER methods[J]. Carbon, 2002,40(9):1521-1531.
[24]
Li G L, Shen B X, Li F K, et al. Elemental mercury removal using biochar pyrolyzed from municipal solid waste[J]. Fuel Processing Technology, 2015,133:43-50.
[25]
Ma J F, Li C T, Zhao L K, et al. Study on removal of elemental mercury from simulated flue gas over activated coke treated by acid[J]. Applied Surface Science, 2015,329:292-300.
[26]
Skodras G, Diamantopoulou Ir, Sakellaropoulos G. P. Role of activated carbon structural properties and surface chemistry in mercury adsorption[J]. Desalination, 2007,210(1):281-286.
[27]
Li H L, Wu C Y, Li L Q, et al. Kinetic modeling of mercury oxidation by chlorine over CeO2-TiO2 catalysts[J]. Fuel, 2013, 113:726-732.
[28]
Lee S J, Seo Y C, Jurng J S, et al. Removal of gas-phase elemental mercury by iodine-and chlorine-impregnated activated carbons[J]. Atmospheric Environment, 2004,38(29):4887-4893.
[29]
Ling L X, Zhao S P, Han P D, et al. Toward predicting the mercury removal by chlorine on the ZnO surface[J]. Chemical Engineering, 2014,244:364-371.
[30]
Tong L, Xu W Q, Qi H, et al. Enhanced effect of O/N groups on the Hg0 removal efficiency over the HNO3-modified activated carbon[J]. Acta Physico-Chimica Sinica, 2015,31:512-518.
[31]
Liu J, Cheney M A, Wu F, et al. Effects of chemical functional groups on elemental mercury adsorption on carbonaceous surfaces[J]. Hazardous Materials, 2011,186:108-113.
[32]
Fuente-Cuesta A, Diaz-Somoano M, Lopez-Anton M A, et al. Biomass gasification chars for mercury capture from a simulated flue gas of coal combustion[J]. Environ. Manage., 2012,98:23-28.
[33]
LEE J Y, Ju Y H, LEE S S, et al. Novel mercury oxidant and sorbent for mercury emissions control from coal-fired power plants[J]. Water, Air, and Soil Pollution:Focus, 2008,8(3/4):333-341.