铜富集菖蒲生物炭对烟气汞去除性能及机制

Abstract
Figure/Table
References
Related Citation (15)

Download: PDF (2273 KB) HTML (1 KB)
Export: BibTeX | EndNote (RIS)

Abstract The biochar containing copper sites (Cu-BC) was prepared by one-step pyrolysis of Cu-enriched Acorus calamus biomass and then utilized for elemental mercury (Hg⁰) removal from the flue gas. The results showed that Cu-BC (Cu-BC500) pyrolyzed at 500℃ exhibited excellent Hg⁰ removal performance (about 99%) at reaction temperature of 100℃. The characterization results including specific surface area analysis (BET), X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectrum (FT-IR) indicated that Cu-BC500 had a relatively high specific surface area, abundant oxygen-containing functional groups and highly dispersed Cu species. XPS and Hg-TPD analyses showed that the mercury adsorbed by Cu-BC500 existed in the forms of weakly bound mercury Cu-O-Hg or copper amalgam at the surface active sites of the biochar samples. Finally, through the life-cycle cost analysis, the cost of Cu-BC500is calculated to be 3.50yuan/kg. Compared with other materials, the preparation of Cu-BC500 is simple and low-costing. The results will provide new ideas for promoting the resource reuse of water restoration plants and mercury emission reduction in coal-fired power plants.

Key words： copper enriched acorus calamus waste utilization biochar flue gas elemental mercury (Hg⁰)

Received: 25 November 2023

PACS:

X701

	Service

	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	LI Hong-hu
	AN Miao
	PENG Xi-yan
	ZHANG Jing-dong
	SUN Yang
	SONG Yong-wei

Cite this article:

LI Hong-hu,AN Miao,PENG Xi-yan等. Performance and mechanism of mercury removal from flue gas by copper-enriched Acorus calamus biochar[J]. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(7): 3646-3654.

URL:

http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2024/V44/I7/3646

[1] 李鸿鹄,彭喜燕,安淼,等.硫酸活化硫酸亚铁絮凝污泥对冶炼烟气中Hg⁰的脱除研究[J]. 中国环境科学, 2023,43(11):5709-5718. Li H H, Peng X Y, An M, et al. Removal of Hg⁰ from smelting flue gas by FeSO₄-flocculated sludge activated with sulfuric acid [J]. China Environmental Science, 2023,43(11):5709-5718.
[2] 王树民,白孝轩,宋畅,等.燃煤电厂大气汞及其他痕量元素排放标准研究[J]. 中国环境科学, 2021,41(4):1949-1958. Wang S M, Bai X X, Song C, et al. Study of atmospheric trace elements emission standards for coal-fired power plants in China [J]. China Environmental Science, 2021,41(4):1949-1958.
[3] Pavlish J H, Sondreal E A, Mann M D, et al. Status review of mercury control options for coal-fired power plants [J]. Fuel Processing Technology, 2003,82:89−165.
[4] Wilcox J, Rupp E, Ying S C, et al. Mercury adsorption and oxidation in coal combustion and gasification processes [J]. International Journal of Coal Geology, 2012,90−91,4.
[5] Scala F, Clack H L. Mercury emissions from coal combustion: Modeling and comparison of Hg capture in a fabric filter versus an electrostatic precipitator [J]. Journal of Hazardous Materials, 2008, 152(2):616-623.
[6] Liu D, Li C,Wu J, et al. Novel carbon-based sorbents for elemental mercury removal from gas streams: A review [J]. Chemical Engineering Journal, 2019,391.
[7] 吕维阳,刘盛余,能子礼超,等.载硫活性炭脱除天然气中单质汞的研究[J]. 中国环境科学, 2016,36(2):382-389. Lv W Y, Liu S Y, Neng Z L C, et al. Remove elemental mercury by sulfur-impregnated activated carbon in natural gas [J]. China Environmental Science, 2016,36(2):382-389.
[8] 吴林虎,吴京懋,王卉.烟气中脱汞吸附剂热再生性能的研究[J]. 发电设备, 2022,36(6):397-401. Wu L H, Wu J M, Wang H, et al. Research on the performance of mercury removal adsorbents in flue gas by thermal regeneration [J]. Generating Equipment, 2022,36(6):397-401.
[9] Yang J, Zhao Y, Zhang J, et al. Removal of elemental mercury from flue gas by recyclable CuCl₂ modified magnetospheres catalyst from fly ash. Part 1. Catalyst characterization and performance evaluation [J]. Fuel, 2016,164:419-428.
[10] Yuan Y, Cao W, Weng W. CuCl₂ immobilized on amino-functionalized MCM-41 and MCM-48 and their catalytic performance toward the vapor-phase oxy-carbonylation of methanol to dimethylcarbonate [J]. Journal of Catalysis, 2004,228(2):311-320.
[11] 周普阳,张新民,张安超,等.Ag-AgIO₃改性BiOI光催化剂湿法脱除气态单质汞[J]. 中国环境科学, 2020,40(11):4703-4711. Zhou P Y, Zhang X M, Zhang A C, et al. Wet process of gaseous Hg⁰ removal by Ag-AgIO₃ modified BiOI photocatalyst [J]. China Environmental Science, 2020,40(11):4703-4711.
[12] 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 mercuryremoval from flue gas using Ag/AgCl photocatalyst under visible light [J]. China Environmental Science, 2017,37(2):503-510.
[13] Hsu C J, Zhao Y Z, Chung A, et al. Novel applications of vacuum distillation for heavy metals removal from wastewater, copper nitrate hydroxide recovery, and copper sulfide impregnated activated carbon synthesis for gaseous mercury adsorption [J]. Science of The Total Environment, 2023,855:158870.
[14] Li H H, Zhang J D, Cao Y X, et al. Role of acid gases in Hg⁰ removal from flue gas over a novel cobalt-containing biochar prepared from harvested cobalt-enriched phytoremediation plant [J]. Fuel Processing Technology, 2020,207:106478.
[15] Shao Y, Fan J, Li J, et al. Removal of elemental mercury from coal combustion flue gas using recyclable Dy modified Mn-Fe mixed oxide nanoparticles [J]. Journal of Environmental Chemical Engineering, 2022,10(5):108493.
[16] 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.
[17] Li H H, Wang S, Wang X, et al. Activity of CuCl₂-modified cobalt catalyst supported on Ti-Ce composite for simultaneous catalytic oxidation of Hg⁰ and NO in a simulated pre-sco process [J]. Chemical Engineering Journal, 2017,316:1103-1113.
[18] Mohamed R M, Ismail A A. Photocatalytic reduction and removal of mercury ions over mesoporous CuO/ZnO S-scheme heterojunction photocatalyst [J]. Ceramics International, 2021,47(7):9659-9667.
[19] 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, 2022,42(1):11-19.
[20] Wang H, Chen H, Hou X, et al. MnO decorated biomass derived carbon based on hyperaccumulative characteristics as advanced electrode materials for high-performance supercapacitors [J]. Diamond and Related Materials, 2023,136:109888.
[21] 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 sorbent [J]. China Environmental Science, 2019,39(6):2336-2343.
[22] 文先彬,张学洪,刘杰.焚烧法和热解法处置Cr超富集植物李氏禾收获物的比较研究[J]. 工业安全与环保, 2018,44(3):73-77. Wen X B, Zhang X H, Liu J. A comparative study on the disposal of harvested products of Cr hyper-accumulator leersia hexandra swartz by incineration and pyrolysis [J]. Industrial Safety and Environmental Protection, 2018,44(3):73-77.
[23] 王胜晓.重金属污染土壤修复植物的厌氧发酵处置与再利用[D]. 南京:南京农业大学, 2023. Wang S X. The anaerobic digestion character of heavy metal contaminated plants and application of it’s biogas residues [D]. Nanjing: Agricultural University of Nanjing, 2023.
[24] 王敏捷,盛光遥,王锐.土壤重金属污染修复植物处置技术进展[J]. 农业资源与环境学报, 2021,38(2):151-159. Wang M J, Sheng G Y, Wang R. Progress in disposal technologies for plants polluted with heavy metals after phytoextraction [J]. The Journal of Agricultural Resources and The Environment, 2021,38(2): 151-159.
[25] Zhou F, Diao Y. Magnetic copper-ferrosilicon composites as regenerable sorbents for Hg⁰ removal [J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2020,590:124447.
[26] Zhao B,Yi H H, Tang X L, et al. Copper modified activated coke for mercury removal from coal-fired flue gas [J]. Chemical Engineering Journal, 2016,286:585-593.
[27] 陈广琳,陈友媛,孙萍,等.滨海区黄花鸢尾的耐盐碱性及氮磷去除效果[J]. 中国环境科学, 2015,35(11):3422-3430. Chen G L, Chen Y Y, Sun P, et al. The Iris Pseudoacorus’ tolerant ability and removal efficiency for nitrogen and phosphorus in saline-alkaline water of coastal region [J]. China Environmental Science, 2015,35(11):3422-3430.
[28] Wang Y, Li H H, He Z, et al. Removal of elemental mercury from flue gas using cobalt-containing biomaterial carbon prepared from contaminated Iris sibirica biomass [J]. ACS Omega, 2020,5(12): 6288-6298.
[29] Yu J, Sun L, Berrueco C, et al. Influence of temperature and particle size on structural characteristics of chars from beechwood pyrolysis [J]. Journal of Analytical and Applied Pyrolysis, 2018,130,127−134.
[30] Xie Y, Li C, Zhao L, et al. Experimental study on Hg⁰ removal from flue gas over columnar MnOx-CeO₂/activated coke [J]. Applied Surface Science. 2015,333:59−67.
[31] 王诗生,张梦梦,盛广宏,等.磁性生物炭吸附水中甲基橙的作用机制-基于密度泛函理论与实验研究[J]. 中国环境科学, 2023,43(9): 4596-4605. Wang S S, Zhang M M, Sheng G H, et al. Adsorption mechanism of methyl orange by using the magnetic biochar —Based on density functional theory and batch adsorption experiment study [J]. China Environmental Science, 2023,43(9):4596-4605.
[32] 刘思强,信欣,杨雯钰,等.不同热解温度BC对BAF处理水产养殖废水的影响机制[J]. 中国环境科学, 2023,43(3):1131-1141. Liu S Q, Xin X, Yang W Y, et al. Influence mechanisms of BC filters of different pyrolysis temperatures on BAFs treating aquaculture wastewater [J]. China Environmental Science, 2023,43(3):1131-1141.
[33] 马锋锋,赵保卫,刁静茹.小麦秸秆生物炭对水中Cd²⁺的吸附特性研究[J]. 中国环境科学, 2017,37(2):551-559. Ma F F, Zhao B W, Diao J R. Adsorptive characteristics of cadmium onto biochar produced from pyrolysis of wheat straw in aqueous solution [J]. China Environmental Science, 2017,37(2):551-559.
[34] 王诗生,赵大唯,章慧娟,等.磁性氮掺杂碳材料活化过硫酸盐降解酸性橙7[J]. 环境科学学报, 2022,42(4):1-10. Wang S S, Zhao D W, Zhang H J, et al. Magnetic N-doped carbonaceous materials activated persulfate for degradation of Acid Orange 7[J]. Acta Scientiae Circumstantiae, 2022,42(4):1-10.
[35] Silva P M M D, Camparotto N G, Figueiredo N T D, et al. Effective removal of basic dye onto sustainable chitosan beads batch and fixed-bed column adsorption, beads stability and mechanism [J]. Sustainable Chemistry and Pharmacy, 2020,18:100348.
[36] 张山,李宁,黄婷,等.污泥基生物炭导电性能的构效机制研究[J]. 中国环境科学, 2023,43(4):1773-1781. Zhang S, Li N, Huang T, Su M X. Structure-activity mechanism of electrical conductivity of sludge-based biochar [J]. China Environmental Science, 2023,43(4):1773-1781.
[37] 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.
[38] 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.
[39] Yang J P, Zhao Y C, Zhang J Y, et al. Removal of elemental mercury from flue gas by recyclable CuCl₂ modified magnetospheres catalyst from fly ash: Part 2. Identification of involved reaction mechanism, Fuel, 2016,167:366-374.
[40] Cao Q, Wang C, Tang D, et al. Enhanced elemental mercury removal in coal-fired flue gas by modified algal waste-derived biochar: Performance and mechanism [J]. Journal of Environmental Management, 2023,325:116427.
[41] 李伟杰,张传明,康金灿,等.镧改性Cu/SiO₂催化剂的乙酸甲酯高效加氢催化性能研究[J]. 燃料化学学报(中英文), 2024,52(2):131- 139. Li W J, Zhang C M, Kang J C,et al. Study on highly efficient hydrogenation of methyl acetate over the lanthanum metal-modified Cu/SiO₂ catalyst [J]. Journal of Chemistry and Technology, 2024,52(2): 131-139.
[42] 董璐.燃煤烟气磁性吸附剂脱汞性能及机理研究[D]. 南京:东南大学, 2021. Dong L. Research on the performance and mechanism of mercury removal by magnetic sorbent from coal-fired flue gas [D]. Nanjing: Southeast China University, 2021.
[43] Liu Y, Yang X, Zhang J, et al. Process simulation of preparing biochar by biomass pyrolysis via aspen plus and its economic evaluation [J]. Waste and Biomass Valorization, 2022,13(5):2609-2622.
[44] Yang Q, Han F, Chen Y, et al. Greenhouse gas emissions of a biomass-based pyrolysis plant in China [J]. Renewable and Sustainable Energy Reviews, 2016,53:1580-1590.
[45] 刘俊伟,田秉晖,张培栋,等.秸秆直燃发电系统的生命周期评价[J]. 可再生能源, 2009,27(5):102-106. Liu J W, Tian B H, Zhang P D, et al. Life cycle assessment on straw directly combustion for power generation system [J]. Renewables, 2009,27(5):102-106.
[46] Harsono S S, Grundman P, Lau L H, et al. Energy balances, greenhouse gas emissions and economics of biochar production from palm oil empty fruit bunches [J]. Resources Conservation and Recycling, 2013,77:108-115.
[47] Liu Y, Zhu Z, Shi J, et al. Facile synthesis and economic analysis of Cu/C catalyst for efficient biodiesel production [J]. International Journal of Energy Research, 2022,46(14):19814-19825.