REMOVAL OF ELEMENTAL MERCURY USING MAGNETIC ADSORBENT PREPARED FROM SLUDGE FLOCCULATED WITH FERROUS SULFATE BY Mn ACTIVATION

WANG Yuan; GUO Huajun; SHAO Yan; LIU Zihao; XIANG Hao; HU Guofeng; LI Honghu; HU Jiangjun

doi:10.13205/j.hjgc.202303010

Volume 41 Issue 3

Mar. 2023

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Article Navigation > ENVIRONMENTAL ENGINEERING > 2023 > 41(3): 74-83

WANG Yuan, GUO Huajun, SHAO Yan, LIU Zihao, XIANG Hao, HU Guofeng, LI Honghu, HU Jiangjun. REMOVAL OF ELEMENTAL MERCURY USING MAGNETIC ADSORBENT PREPARED FROM SLUDGE FLOCCULATED WITH FERROUS SULFATE BY Mn ACTIVATION[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(3): 74-83. doi: 10.13205/j.hjgc.202303010

Citation:

WANG Yuan, GUO Huajun, SHAO Yan, LIU Zihao, XIANG Hao, HU Guofeng, LI Honghu, HU Jiangjun. REMOVAL OF ELEMENTAL MERCURY USING MAGNETIC ADSORBENT PREPARED FROM SLUDGE FLOCCULATED WITH FERROUS SULFATE BY Mn ACTIVATION[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(3): 74-83. doi: 10.13205/j.hjgc.202303010

Citation:

WANG Yuan, GUO Huajun, SHAO Yan, LIU Zihao, XIANG Hao, HU Guofeng, LI Honghu, HU Jiangjun. REMOVAL OF ELEMENTAL MERCURY USING MAGNETIC ADSORBENT PREPARED FROM SLUDGE FLOCCULATED WITH FERROUS SULFATE BY Mn ACTIVATION[J]. ENVIRONMENTAL ENGINEERING , 2023, 41(3): 74-83. doi: 10.13205/j.hjgc.202303010

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REMOVAL OF ELEMENTAL MERCURY USING MAGNETIC ADSORBENT PREPARED FROM SLUDGE FLOCCULATED WITH FERROUS SULFATE BY Mn ACTIVATION

doi: 10.13205/j.hjgc.202303010

1. WISDRI City Environment Protection Engineering Co., Ltd, Wuhan 430200, China;
2. School of Information and Safety Engineering, Zhongnan University of Economics and Law, Wuhan 430073, China;
3. School of Resource and Environmental Sciences, Wuhan University, Wuhan 430079, China

Received Date: 2022-04-21
Available Online: 2023-05-26
Publish Date: 2023-03-01

Abstract

Abstract

In this work, ferrous sulfate-flocculated sewage sludge (SFS) was activated by Mn(NO₃)₂ and then pyrolyzed to obtain magnetic adsorbent, which was adopted to remove elemental mercury (Hg⁰) from flue gas. Results showed that 1) O₂ produced by the thermal decomposition of Mn(NO₃)₂ promoted the decomposition of FeC_<em>x during primary pyrolysis of sludge, and that was conducive to the formation of high-valent metal oxides such as Mn⁴⁺and Fe³⁺. The gas produced by the decomposition of Mn(NO₃)₂ also showed the effect of pore expansion. With the addition of 10% Mn(NO₃)₂, the specific surface area of the adsorbent reached the maximum (88.5 m²/g), but when the Mn(NO₃)₂ amount continued to rise, it would produce many crystalline substances and then decreased the specific surface area of the adsorbent. 2) Mn₁₀-SFS showed a maximum mercury removal efficiency of 92.7% at the reaction temperature of 150 ℃. 3) O₂ could effectively supplement the active oxygen in the adsorbent, promoting the removal of Hg⁰, and presence of NO and a low SO₂ concentration enhanced Hg⁰ removal, while H₂O vapor and a high concentration of SO₂ inhibited it. The Hg⁰ adsorption and desorption experiment showed that the adsorbent of Mn₁₀-SFS exhibited good renewable recycling performance and stability. After Hg⁰ capture and regeneration for 5 cycles, the removal efficiency of the adsorbent was not notably degraded.
- sludge,
- adsorbent,
- coal-fired flue gas,
- mercury removal

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References(29)

References

[1]	YANG Y J, LIU J, WANG Z. Reaction mechanisms and chemical kinetics of mercury transformation during coal combustion[J]. Progress in Energy and Combustion Science, 2020, 79:100844.
[2]	YANG S J, GUO Y F, YAN N Q, et al. Remarkable effect of the incorporation of titanium on the catalytic activity and SO₂ poisoning resistance of magnetic Mn-Fe spinel for elemental mercury capture[J]. Applied Catalysis B:Environmental, 2011, 101(3/4):698-708.
[3]	姬丽琴, 齐永新, 周林成, 等. 磁性微/纳米材料吸附环境污染物的研究进展[J]. 化工新型材料, 2011, 39(11):32-35.
[4]	DONG L, HUANG Y J, CHEN H, et al. Magnetic γFe₂O₃loaded attapulgite sorbent for Hg⁰ removal in coal-fired flue gas[J]. Energy & Fuels, 2019, 33(8):7522-7533.
[5]	ZENG X B, XU Y, ZHANG B, et al. Elemental mercury adsorption and regeneration performance of sorbents FeMnO_x enhanced via non-thermal plasma[J]. Chemical Engineering Journal, 2017, 309:503-512.
[6]	YANG S J, GUO Y F, YAN N Q, et al. Nanosized cation-deficient Fe-Ti spinel:a novel magnetic sorbent for elemental mercury capture from flue gas[J]. ACS Applied Materials & Interfaces, 2011, 3(2):209-217.
[7]	YANG S J, GUO Y F, YAN N Q, et al. Capture of gaseous elemental mercury from flue gas using a magnetic and sulfur poisoning resistant sorbent Mn/γ-Fe₂O₃ at lower temperatures[J]. Journal of Hazardous Materials, 2011, 186(1):508-515.
[8]	YANG S J, YAN N Q, GUO Y F, et al. Gaseous elemental mercury capture from flue gas using magnetic nanosized (Fe_3-xMn_x)_1-δO₄[J]. Environmental Science & Technology, 2011, 45(4):1540-1546.
[9]	ZHANG Z H, WU J, LI B, et al. Removal of elemental mercury from simulated flue gas by ZSM-5 modified with Mn-Fe mixed oxides[J]. Chemical Engineering Journal, 2019, 375:121946.
[10]	林子增,黄瑛,乔红杰,等. 城市污水厂污泥化学调理深度脱水技术述评[J]. 应用化工, 2016, 45(6):1159-1162.
[11]	YANG X, XU G R, YU H R, et al. Preparation of ferric-activated sludge-based adsorbent from biological sludge for tetracycline removal[J]. Bioresource Technology, 2016, 211:566-573.
[12]	WANG Y, LI H H, HE Z, et al. Removal of elemental mercury from flue gas using the magnetic Fe-containing carbon prepared from the sludge flocculated with ferrous sulfate[J]. Environmental Science and Pollution Research, 2020, 27:30254-30264.
[13]	WANG Y, LI H H, SHAO Y, et al. Removal of elemental mercury using magnetic Fe-containing carbon prepared from sludge flocculated with ferrous sulfate by zinc chloride activation[J]. Journal of the Energy Institute, 2021, 98:98-106.
[14]	YANG Y J, LIU J, WANG Z, et al. Interface reaction activity of recyclable and regenerable Cu-Mn spinel-type sorbent for Hg⁰ capture from flue gas[J]. Chemical Engineering Journal, 2019, 372:697-707.
[15]	吕浩. 活性炭喷射耦合除尘器协同脱除燃煤烟气有机污染物/汞/CPM研究[D]. 南京:东南大学,2021.
[16]	LIAO Y, CHEN D, ZOU S J, et al. A recyclable naturally derived magnetic pyrrhotite for elemental mercury recovery from the flue gas[J]. Environmental Science & Technology, 2016, 50:10562-10569.
[17]	杨建平. 可循环再生磁珠吸附剂脱汞及其反应机理研究[D]. 武汉:华中科技大学, 2017.
[18]	LI H H, WANG S K, WANG X, et al. FeCl₃-modified Co-Ce oxides catalysts for mercury removal from coal-fired flue gas[J]. Chemical Papers, 2017, 71(12):2545-2555.
[19]	XU Y, LUO G Q, PANG Q C, et al. Adsorption and catalytic oxidation elemental mercury over regenerable magnetic Fe-Ce mixed oxides modified by non-thermal plasma treatment[J]. Chemical Engineering Journal, 2019, 358:1454-1463.
[20]	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, 547-56.
[21]	LI H L, WU C Y, LI Y, et al. Impact of SO₂ on elemental mercury oxidation over CeO₂-TiO₂ catalyst[J]. Chemical Engineering Journal, 2013, 219:319-326.
[22]	LI H H, WANG S K, WANG X, et al. Catalytic oxidation of Hg⁰ in flue gas over Ce modified TiO₂ supported Co-Mn catalysts:characterization, the effect of gas composition and co-benefit of NO conversion[J]. Fuel, 2017, 202:470-482.
[23]	SHAN Y, YANG W, LI Y, et al. Reparation of microwave-activated magnetic bio-char adsorbent and study on removal of elemental mercury from flue gas[J]. Science of the Total Environment, 2019, 697:134049.
[24]	YANG J P, ZHAO Y C, LIANG S F, et al. Magnetic iron-manganese binary oxide supported on carbon nanofiber (Fe_3-xMn_xO₄/CNF) for efficient removal of Hg⁰ from coal combustion flue gas[J]. Chemical Engineering Journal, 2018, 334:216-224.
[25]	ZHANG A C, ZHANG Z H, CHEN J J, et al. Effect of calcination temperature on the activity and structure of MnO_x/TiO₂ adsorbent for Hg⁰ removal[J]. Fuel Processing Technology, 2015, 135:25-33.
[26]	YANG J P, ZHAO Y, MA S, et al. Mercury removal by magnetic biochar derived from simultaneous activation and magnetization of sawdust[J]. Environmental Science & Technology 2016, 50(21):12040-12047.
[27]	DUAN X L, YUAN C G, JING T T, et al. Removal of elemental mercury using large surface area micro-porous corn cob activated carbon by zinc chloride activation[J]. Fuel, 2019, 239:830-840.
[28]	ZOU S J, LIAO Y, XIONG S, et al. H₂S-modified Fe-Ti spinel:a recyclable magnetic sorbent for recovering gaseous elemental mercury from flue gas as a co-benefit of wet electrostatic precipitators[J]. Environment Science & Technology, 2017, 51(6):3426-3434.
[29]	ZHOU F S, DIAO Y F, Magnetic copper-ferrosilicon composites as regenerable sorbents for Hg⁰ removal[J]. Colloids and Surface A, 2020, 590:124447.