硫酸活化硫酸亚铁絮凝污泥对冶炼烟气中Hg<sup>0</sup>的脱除研究

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Abstract A kind of adsorbent (SS_XT_Y) with excellent performance on efficiently capturing Hg⁰ in smelting flue gas was prepared from ferrous sulfate-flocculated sludge with sulfuric acid activation. H₂SO₄ activation could improve the adsorbent pore structure and increase the active surface oxygen/sulfur species, thus leading to the enhanced mercury removal activity of the adsorbent. Moreover, the SO₂ resistance of the adsorbent was greatly improved, which could effectively overcome the inhibition effect of SO₂ in actual working conditions. Pyrolysis temperature and H₂SO₄ addition ratio showed significant effects on the mercury removal activity of adsorbent. SS₂₅T₆₅₀(H₂SO₄ addition ratio of 0.25 and pyrolysis temperature of 650℃) exhibited the highest mercury removal efficiency (95.4%). Using flocculated sludge to produce mercury adsorbent not only reduces the adsorbent cost, but also provides a potential way for the resource utilization of flocculated sludge. SS_XT_Y has the advantages of simple preparation method, low cost, excellent SO₂ resistance and prominent mercury removal performance, thus showing promising application prospects.

Key words： sulfuric acid activation ferrous sulfate-flocculated sludge smelting flue gas elemental mercury mechanism

Received: 20 March 2023

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X511

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	LI Hong-hu
	PENG Xi-yan
	AN Miao
	LI Jia-yi
	CAO Yan-xiao

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LI Hong-hu,PENG Xi-yan,AN Miao等. Removal of Hg⁰ from smelting flue gas by FeSO₄-flocculated sludge activated with sulfuric acid[J]. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(11): 5709-5718.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2023/V43/I11/5709

[1]	吴清茹,王书肖,王玉晶.中国有色金属冶炼行业大气汞排放趋势预测[J]. 中国环境科学, 2017,37(7):2401-2413. Wu Q R, Wang S X, Wang Y J. Projections of atmospheric mercury emission trends in China's nonferrous metalsing industry [J]. China Environmental Science, 2017,37(7):2401-2413.
[2]	吴晓慧,徐丽笑,齐剑川,等.中国大气汞排放变化的社会经济影响因素[J]. 中国环境科学, 2021,41(4):1959-1969. Wu X H, Xu L X, Qi J C, et al. Socioeconomic factors influencing atmospheric mercury emission changes in China [J]. China Environmental Science, 2021,41(4):1959-1969.
[3]	Pirrone N, Cinnirella S, Feng X, et al. Global mercury emissions to the atmosphere from anthropogenic and natural sources [J]. Atmospheric Chemistry and Physics, 2010,10(13):5951-5964.
[4]	郑逸武,段钰锋,汤红健,等.燃煤烟气污染物控制装置协同脱汞特性研究[J]. 中国环境科学, 2018,38(3):862-870. Zheng Y W, Duan Y F, Tang H J, et al. Characteristics of the existing air pollutant control devices on Hg synergistic removal in a coal-fired power plant [J]. China Environmental Science, 2018,38(3):862-870.
[5]	邢微波,路好,张安超,等.Ag/AgCl可见光催化剂湿法脱除烟气中单质汞[J]. 中国环境科学, 2017,37(2):503-510. Xing W B, Lu H, Zhang A C, et al. Wet process of elemental mercury removal from flue gas using Ag/AgCl photocatalyst under visible light [J]. China Environmental Science, 2017,37(2):503-510.
[6]	Wang C, Qin R Y, Zhang X F, et al. Safe disposal of deactivated commercial selective catalytic reduction catalyst (V2O5-MoO3/TiO2) as a low-cost and regenerable sorbent to recover gaseous elemental mercury in smelting ﬂue gas [J]. Journal of Hazardous Materials, 2021, 406:124744.
[7]	Kong L N, Zou S J, Mei J, et al. Outstanding resistance of H2S-modifed Cu/TiO2 to SO2 for capturing gaseous Hg0from nonferrous metal smelting ﬂue gas:performance and reaction mechanism [J]. Environmental Science & Technology, 2018,52(17):10003-10010.
[8]	马永鹏.有色金属冶炼烟气中汞的排放控制与高效回收技术研究[D]. 上海:上海交通大学, 2014. Ma Y P. Study on mercury emission control and reclaim technology from non-ferrous metal smelting flue gas [D]. Shanghai:Shanghai Jiao Tong University, 2014.
[9]	Liu Z L, Peng B, Chai L Y, et al. Selective removal of elemental mercury from high-concentration SO2 ﬂue gas by thiourea solution and investigation of mechanism [J]. Industrial & Engineering Chemistry Research, 2017,56(15):4281-4287.
[10]	李子良,徐志峰.有色金属冶炼烟气中单质汞脱除研究现状[J]. 有色金属科学与工程, 2020,11(2):20-26. Li Z L, Xu Z F. Research status of elemental mercury removal from flue gas in non-ferrous metals production [J]. Nonferrous Metals Science and Engineering, 2020,11(2):20-26.
[11]	Xu W, Hussain A, Liu X Y. A review on modification methods of adsorbents for elemental mercury from flue gas [J]. Chemical Engineering Journal, 2018,346:692-711.
[12]	Sano A, Takaoka M, Shiota K. Vapor-phase elemental mercury adsorption by activated carbon co-impregnated with sulfur and chlorine [J]. Chemical Engineering Journal, 2017,315:598-607.
[13]	Ma Y P, Mu B L, Zhang X J, et al. Hierarchical Ag-SiO2@Fe3O4 magnetic composites for elemental mercury removal from non-ferrous metal smelting flue gas [J]. Journal of Environmental Sciences, 2019, 79:111-120.
[14]	Han L, He X, Yue C, et al. Fe doping Pd/AC sorbent efficiently improving the Hg0 removal from the coal-derived fuel gas [J]. Fuel, 2016,182:64-72.
[15]	吴响,段钰锋,姚婷等.Ce-Mn/TiO2吸附剂的脱汞性能及抗SO2特性[J]. 中国环境科学, 2019,39(6):2336-2343. Wu X, Duan Y F, Yao T, et al. Mercury removal performance and SO2 resistance of Ce-Mn/TiO2 adsorbent [J]. China Environmental Science, 2019,39(6):2336-2343.
[16]	邱磊,郭磊,韩金池,等.改性镍铝催化剂氧化零价汞及抗氨干扰机理[J]. 中国环境科学, 2022,42(1):11-19. Qiu L, Guo L, Han J C, et al. Hg0oxidation of modified Ni-Al catalysts and its anti-ammonia interference mechanism [J]. China Environmental Science, 2019,39(6):2336-2343.
[17]	Xu Y, Luo G Q, Pang Q C, et al. Adsorption and catalytic oxidation of elemental mercury over regenerable magnetic Fe-Ce mixed oxides modified by non-thermal plasma treatment [J]. Chemical Engineering Journal, 2019,358:1454-1463.
[18]	刘东京,张禛,吴江.载铜氮化碳纳米片对单质汞的吸附脱除特性[J]. 中国环境科学, 2019,39(5):1862-1868. Liu D J, Zhang Z, Wu J. Adsorption removal of elemental mercury on Cu-loaded carbon nitride nanosheet [J]. China Environmental Science, 2019,39(5):1862-1868.
[19]	Liu D J, Li C, W J, et al. Novel carbon-based sorbents for elemental mercury removal from gas streams:A review [J]. Chemical Engineering Journal, 2020,391:123514.
[20]	Ralston N. Nano-selenium captures mercury [J]. Nature Nanotechnology, 2008,3(11):648.
[21]	Yang Z Q, Li H L, Yang J P, et al. Nanosized copper selenide functionalized zeolitic imidazolate framework-8(CuSe/ZIF-8) for efficient immobilization of gas-phase elemental mercury [J]. Advanced Functional Materials, 2019,29(17):1807191.
[22]	Liu W, Xu H M, Liao Y, et al. 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.
[23]	Yang S, Wang D L, Liu H, et al. Highly stable activated carbon composite material to selectively capture gas-phase elemental mercury from smelting flue gas:Copper polysulfide modification [J]. Chemical Engineering Journal, 2019,358:1235-1242.
[24]	Zhang Y S, Mei D Q, Wang T, et al. In-situ capture of mercury in coal-fired power plants using high surface energy fly ash [J]. Environmental Science & Technology, 2019,53(13):7913-7920.
[25]	Liu T, Xiong Z, Ni P, et al. Review on adsorbents in elemental mercury removal in coal combustion flue gas, smelting flue gas and natural gas [J]. Chemical Engineering Journal, 2023,454(1):140095.
[26]	Chen Y C, Rong H, Zhang J D, et al. Investigation of a carbon-based sorbent prepared from FeSO4-flocculated sludge for elemental mercury removal from syngas [J]. Waste and Biomass Valorization, 2022,13(2):1323-1337.
[27]	Liao Y, Chen D, Zou S J, et al. Recyclable naturally derived magnetic pyrrhotite for elemental mercury recovery from flue gas [J]. Environmental Science & Technology, 2016,50(19):10562-10569.
[28]	Dong L, Huang Y J, Chen H, et al. Magnetic γ-Fe2O3 loaded attapulgite sorbent for Hg0 removal in coal-fired flue gas [J]. Energy & Fuels, 2019,32(8):7522-7533.
[29]	Liu Z L, Li Z L, Xie X F, et al. Development of recyclable iron sulfide/selenide microparticles with high performance for elemental mercury capture from smelting flue gas over a wide temperature range [J]. Environmental Science & Technology, 2020,54(1):604-612.
[30]	Wang C, Zhang X F, Mei J, et al. Novel synergistic effect of Fe and Mo in FeMoSx/TiO2 for recovering high concentrations of gaseous Hg0 from smelting flue gas:Reaction mechanism and kinetics [J]. Environmental Science & Technology, 2019,54(1):586-594.
[31]	Dong L, Huang Y J, Chen H, et al. Magnetic γ‑Fe2O3‑loaded attapulgite sorbent for Hg0 removal in coal-fired flue gas [J]. Energy & Fuels, 2019,32(8):7522-7533.
[32]	李子良.改性铁硫化物对冶炼烟气中单质汞的脱除性能研究[D]. 赣州:江西理工大学, 2021. Li Z L. Removal of elemental mercury from smelting flue gas by modified iron sulfide [D]. Ganzhou:Jiangxi University of Science and Technology, 2021.
[33]	张永强,贾里,乔晓磊,等.腐殖酸定向修饰Ce-Co铁基生物焦汞吸附机理[J]. 中国环境科学, 2021,41(12):5522-5530. Zhang Y Q, Jia L, Qiao X L, et al. The absorption mechanism of humic acid directional modification Ce-Co modified iron-based biochar mercury [J]. China Environmental Science, 2021,41(12):5522-5530.
[34]	Wang X, Zhang P, Wang C, et al. Metal-rich hyperaccumulator-derived biochar as an efficient persulfate activator:Role of intrinsic metals (Fe, Mn and Zn) in regulating characteristics, performance and reaction mechanisms [J]. Journal of hazardous materials, 2022,424:127225.
[35]	Li H H, Peng X Y, An M, et al. Negative effect of SO2 on mercury removal over catalyst/sorbent from coal-fired flue gas and its coping strategies:A review [J]. Chemical Engineering Journal, 2023,455:140751.
[36]	黄瑞,杨阳,徐文青,等.金属硫化物吸附剂脱除烟气汞研究进展[J]. 化工进展, 2020,39(12):5243-5251. Huang R, Yang Y, XU W Q, et al. Research progress of metal sulfide adsorbents for removing mercury in flue gas [J]. Chemical Industry and Engineering Progress, 2020,39(12):5243-5251.
[37]	沈畅,王卉,沈昊天,等.烟气抗硫脱汞材料的研究进展[J]. 中南大学学报(自然科学版), 2021,52(1):133-143. Shen C, Wang H, Shen H T, et al. Research progress on flue gas mercury removal materials with SO2 resistance [J]. Journal of Central South University (Science and Technology), 2021,52(1):133-143.
[38]	Wang A, Chen W, Liu S Y, Layered porous carbon material derived from food residues and its application for elemental mercury adsorption in flue gas [J]. Fuel, 2023,335:126876.
[39]	Li H H, Zhang J D, Cao Y X, et al. Capture of elemental mercury from flue gas over a magnetic and sulfur-resistant sorbent prepared from Fe-containing sewage sludge activated with sulfuric aid [J]. Fuel, 2021,300:120938.
[40]	汪远,郭华军,邵雁等.Mn活化铁盐絮凝污泥制备磁性吸附剂脱除烟气中Hg0 [J]. 环境工程, 2023,41(3):74-83. Wang Y, Guo H J, Shao Y, et al. Removal of elemental mercury using magnetic adsorbent prepared form sludge flocculated with ferrous sulfate by Mn activation [J]. Environmental Engineering, 2023,41(3):74-83.
[41]	Ding Z, Yang C, Zhang H, et al. New utilizations of natural CuFeS2 as the raw material of Cu smelting for recovering Hg0 from Cu smelting flue gas [J]. Fuel, 2023,341:126997.
[42]	Cao Q H, Wang C, Tang D Y, et al. Enhanced elemental mercury removal in coal-fired flue gas by modified algal waste-derived biochar:Performance and mechanism [J]. Journal of Environment Management, 2023,325:116427.