留言板

尊敬的读者、作者、审稿人, 关于本刊的投稿、审稿、编辑和出版的任何问题, 您可以本页添加留言。我们将尽快给您答复。谢谢您的支持!

姓名
邮箱
手机号码
标题
留言内容
验证码

臭氧氧化-生物炭吸附体系协同脱硫脱硝除汞研究

严永桂 毛中建 罗津晶 杜如鹏 林家璇

严永桂, 毛中建, 罗津晶, 杜如鹏, 林家璇. 臭氧氧化-生物炭吸附体系协同脱硫脱硝除汞研究[J]. 燃料化学学报, 2020, 48(12): 1452-1460.
引用本文: 严永桂, 毛中建, 罗津晶, 杜如鹏, 林家璇. 臭氧氧化-生物炭吸附体系协同脱硫脱硝除汞研究[J]. 燃料化学学报, 2020, 48(12): 1452-1460.
YAN Yong-gui, MAO Zhong-jian, LUO Jin-jing, DU Ru-peng, LIN Jia-xuan. Simultaneous removal of SO2, NOx and Hg0 by O3 oxidation integrated with bio-charcoal adsorption[J]. Journal of Fuel Chemistry and Technology, 2020, 48(12): 1452-1460.
Citation: YAN Yong-gui, MAO Zhong-jian, LUO Jin-jing, DU Ru-peng, LIN Jia-xuan. Simultaneous removal of SO2, NOx and Hg0 by O3 oxidation integrated with bio-charcoal adsorption[J]. Journal of Fuel Chemistry and Technology, 2020, 48(12): 1452-1460.

臭氧氧化-生物炭吸附体系协同脱硫脱硝除汞研究

基金项目: 

厦门市科技计划 3502z20173014

详细信息
  • 本文的英文电子版由Elsevier出版社在ScienceDirect上出版(http://www.sciencedirect.com/science/journal/18725813).
  • 中图分类号: X511

Simultaneous removal of SO2, NOx and Hg0 by O3 oxidation integrated with bio-charcoal adsorption

Funds: 

the Science and Technology Planning Project of Xiamen 3502z20173014

More Information
  • 摘要: 以O3为氧化剂,玉米生物炭和椰壳活性炭为吸附剂,开展同时脱硫脱硝除汞研究。研究考察了温度、O3/NO和吸附时间对玉米/椰壳炭脱硫脱硝除汞效率的影响,并对玉米/椰壳炭进行表征分析。结果表明,NO和Hg0氧化率随O3/NO升高而升高,SO2氧化率则先升高后略微降低;温度升高抑制NO氧化但促进Hg0和SO2氧化;在140 ℃下,当O3/NO为1.4时,NO、Hg0和SO2氧化率分别达99%、78.6%和3.5%,随O3/NO从0.4升至1.4,玉米炭对NOx脱除效率从4.6%提升至93%,椰壳炭从4.5%提升至79%。玉米/椰壳炭会还原部分NO2造成出口NO浓度上升,但玉米炭的NOx吸附性能较椰壳炭强,而椰壳炭对Hg0和SO2的吸附性能较强。椰壳炭较玉米炭具有更强的物理吸附能力;玉米炭表面含氧官能团C-O和C=O的相对含量较椰壳炭高,而COOH和O=C-O相对含量较椰壳炭低。
    1)  本文的英文电子版由Elsevier出版社在ScienceDirect上出版(http://www.sciencedirect.com/science/journal/18725813).
  • 图  1  实验装置示意图

    Figure  1.  Adsorption experimental apparatus

    图  2  O3/NO物质的量比对NO、SO2和Hg0氧化率的影响

    Figure  2.  Influences of O3/NO molar ratio on the oxidation efficiency of NO, SO2 and Hg0

    图  3  O3/NO物质的量比对NOx、SO2和Hg0去除效率的影响

    Figure  3.  Influence of O3/NO molar ratio on the removal efficiency of NOx, SO2 and Hg0

    图  4  不同O3/NO物质的量比下炭吸附后出口烟烟气中的NO、NO2质量浓度

    Figure  4.  Concentrations of NO and NO2 in flue gas after carbon adsorption at different O3/NO molar ratios

    图  5  玉米炭对NOx、SO2和Hg0的吸附

    Figure  5.  Adsorption curve of NOx, SO2 and Hg0 on corn charcoal

    图  6  椰壳炭对NOx、SO2和Hg0的吸附

    Figure  6.  Adsorption curve of NOx, SO2 and Hg0 on coconut shell charcoal

    图  7  椰壳炭的SEM照片

    Figure  7.  SEM image of coconut shell charcoal

    图  8  玉米炭的SEM照片

    Figure  8.  SEM image of corn charcoal

    图  9  椰壳炭(a)、玉米炭(b)的XPS全谱谱图

    Figure  9.  XPS full spectrum

    (a): the coconut shell charcoal; (b): the corn charcol

    表  1  样品的元素分析

    Table  1.   Elemental composition of the sample

    Sample Uitimate analysis w/% O/C N/C (O+N)/C
    C N H S O
    CS 79.984 0.249 1.258 0.667 17.842 0.223 0.003 0.226
    CR 63.254 1.582 1.698 0.268 33.198 0.525 0.025 0.549
    下载: 导出CSV

    表  2  C 1s、O 1s和N 1s含量及比例

    Table  2.   Content and proportion of C 1s, O 1s and N 1s obtained from XPS

    Sample C 1s O 1s N 1s O/C N/C
    CS 91.38 7.44 0.58 0.081 0.006
    CR 81.71 14.53 1.61 0.178 0.019
    下载: 导出CSV

    表  3  样品的C 1s分峰

    Table  3.   C 1s peak fitting results of samples

    Sample Peak label Peak position /eV Functional group Content
    CS C1 284.8 C-C 0.554
    C2 286.1 C-O 0.228
    C3 288.5 C=O 0.067
    C4 290.6 COOH 0.151
    CR C1 284.8 C-C 0.599
    C2 286.1 C-O 0.267
    C3 288.5 C=O 0.115
    C4 290.6 COOH 0.100
    下载: 导出CSV

    表  4  样品的O 1s分峰

    Table  4.   O 1s peak fitting results of samples

    Sample Peak label Peak position /eV Functional group Content
    CS O1 531.5 C=O 0.171
    O2 532.5 C-O 0.532
    O3 533.3 O=C-O 0.098
    O4 534.2 COOH 0.199
    CR O1 531.5 C=O 0.284
    O2 532.5 C-O 0.621
    O3 533.3 O=C-O 0.039
    O4 534.2 COOH 0.066
    下载: 导出CSV
  • [1] SARBASSOV Y, DUAN L, JEREMIAS M, MANOVIC V, EDWARD J. SO3 formation and the effect of fly ash in a bubbling fluidised bed under oxy-fuel combustion conditions[J]. Fuel Process Technol, 2017, 167(1): 314-21.
    [2] ZHENG Y, JENSEN A D, WINDELIN C, JENSEN F. Review of technologies for mercury removal from flue gas from cement production processes[J]. Prog Energy Combust Sci, 2012, 38 (5): 599-629.
    [3] JIN D S, DESHWAL B R, PARK Y S, LEE H K. Simultaneous removal of SO2 and NO by wet scrubbing using aqueous chlorine dioxide solution[J]. J Hazaed Mater, 2006, 135(1/3): 412-417.
    [4] 周国民, 唐建成, 胡振广, 赵海军, 龚家猷.燃煤锅炉SNCR脱硝技术应用研究[J].电站系统工程, 2010, 26(1): 18-21.

    ZHOU Guo-min, TANG Jian-cheng, HU Zhen-guang, ZHAO Hai-jun, GONG Jia-you. Application eesearch of SNCR technology in the pulverized-coal fired boiler[J]. Pwr Sy Eng, 2010, 26(1): 18-21.
    [5] 顾卫荣, 周明吉, 马薇.燃煤烟气脱硝技术的研究进展[J].化工进展, 2012, 31(9): 2084-2092.

    GU Wei-rong, ZHOU Ming-ji, MA Wei. Technology status and analysis on coal-fired flue gas denitrification[J]. Chem Ind Eng Prog, 2012, 31(9): 2084-2092.
    [6] 张杰儒, 罗津晶, 牛强.垃圾焚烧烟气汞的治理技术与评价[J].环境卫生工程, 2012, 20(5): 34-36.

    ZHANG Jie-ru, LUO Jin-jing, NIU Qiang. Control technologies and evaluation of mercury in flue gas of waste incineration[J]. Environ Sanitation Eng, 2012, 20(5): 34-36.
    [7] ZHANG B, XU P, QIU Y, YU Q, MA J J, WU H, LUO G Q, XU M H, YAO H. Increasing oxygen functional groups of activated carbon with non-thermal plasma to enhance mercury removal efficiency for flue gases[J]. Chem Eng J, 2015, 263: 1-8.
    [8] WANG L, ZHAO W R, WU Z B. Simultaneous absorption of NO and SO2 by FeEDTA combined with Na2SO3 solution[J]. Chem Eng J, 2007, 132(1/3): 227-232.
    [9] ZHAO Y, XU P Y, FU D, HUANG J J, YU H H. Experimental study on simultaneous desulfurization and denitrification based on highly active absorbent[J]. J Environ Sci, 2006, 18(2): 281-286.
    [10] CHIU C H, HSI H C, LIN H P. Multipollutant control of Hg/SO2/NO from coal-combustion flue gases using transition metal oxide-impregnated SCR catalysts[J]. Catal Today, 2015, 245: 2-9.
    [11] ZHANG S, ZHAO Y, WANG Z, ZHANG J Y, WANG L L, ZHENG C G. Integrated removal of NO and mercury from coal combustion flue gas using manganese oxides supported on TiO2[J]. J Environ Sci, 2016, 53 (3): 141-150.
    [12] ZHANG S B, ZHANG Q Z, ZHAO Y C, YANG J P, XU Y, ZHANG J Y. Enhancement of CeO2 modified commercial SCR catalyst for synergistic mercury removal from coal combustion flue gas[J]. Rsc Adv, 2020, 10: 25325-25338.
    [13] 温正城, 王智化, 杨卫娟, 周俊虎, 岑可法.臭氧在烟气中氧化零价汞的机理研究[J].浙江大学学报(工学版), 2009, 43(9): 1625-1631.

    WEN Zheng-cheng, WANG Zhi-hua, YANG Wei-juan, ZHOU Jun-hu, CEN Ke-fa. Mechanism investigation on oxidization of Hg0 by ozone in flue gas[J]. J Zhejiang Univ (Eng Sci), 2009, 43(9): 1625-1631.
    [14] 王智化, 周俊虎, 温正城, 张彦威, 岑可法.利用臭氧同时脱硫脱硝过程中NO的氧化机理研究[J].浙江大学学报(工学版), 2007, 41(5): 765-769.

    WANG Zhi-hua, ZHOU Jun-hu, WEN Zheng-cheng, ZHANG Yan-wei, CEN Ke-fa. Mechanism investigation on NO oxidization during NOx and SO2 simultaneous removal process by Ozone[J]. J Zhejiang Univ (Eng Sci), 2007, 41(5): 765-769.
    [15] 张明慧, 马强, 徐超群, 朱燕群, 周俊虎.臭氧氧化结合湿法喷淋对玻璃窑炉烟气同时脱硫脱硝实验研究[J].燃料化学学报, 2015, 43(1): 88-93.

    ZHANG Ming-hui, MA Qiang, XU Chao-qun, ZHU Yan-qun, ZHOU Jun-hu. Simultaneous removal of NOx and SO2 from glass furnace flue gas by ozone oxidation and spray tower[J]. J Fuel Chem Technol, 2015, 43(1): 88-93.
    [16] 张瑞, 张佳, 郭少鹏, 刘勇弟, 鲁军.臭氧氧化同时脱除烟气中NO和SO2的研究[J].化学世界, 2015, (3): 158-161.

    ZHANG Rui, ZHANG Jia, GUO Shao-peng, LIU Yong-di, LU Jun. Study on simultaneous removal of NO and SO2 from flue gas by ozone oxidation[J]. Chem World, 2015, (3): 158-161.
    [17] 王智化, 周俊虎, 魏林生, 温正城, 岑可法.用臭氧氧化技术同时脱除锅炉烟气中NOx及SO2的试验研究[J].中国电机工程学报, 2007, 27(11): 1-5.

    WANG Zhi-hua, ZHOU Jun-hu, WEI Lin-sheng, WEN Zheng-cheng, CEN Ke-fa. Experimental research for the simultaneous removal of NOx and SO2 in flue gas by O3[J]. Proc CSEE, 2007, 27(11): 1-5.
    [18] 牛强, 罗津晶, 郑锦森, 王巍, 汪可涛.臭氧氧化技术同时脱除烟气中NO和SO2的试验研究[J].广东化工, 2020, 12(47): 159-161.

    NIU Qiang, LUO Jin-jing, ZHENG Jin-sen, WANG Wei, WANG Ke-tao. Experimental research for the simultaneous removal of NO and SO2 in flue gas[J]. Guangdong Chem Ind, 2020, 12(47): 159-161.
    [19] 李兵, 张立强, 蒋海涛, 王志强, 马春元.活性炭孔隙结构和表面化学性质对吸附氧化NO的影响[J].煤炭学报, 2011, 36(11): 1906-1910.

    LI Bing, ZHANG Li-qiang, JIANG Hai-tao, WANG Zhi-qiang, MA Chun-yuan. Influence of activated carbon pore structure and surface chemical properties on the adsorption and oxidation of NO[J]. J China Coal Soc, 2011, 36(11): 1906-1910.
    [20] ZHANG W J, RABIEI S, BAGREEV A, ZHUANG M S, RASOULI F. Study of NO adsorption on activated carbons[J]. Appl Catal B: Environ, 2008, 83(1/2): 63-71.
    [21] 张波文, 唐晓龙, 易红宏, 赵顺征, 左嫣然, 王志祥, 高凤雨.改性活性炭吸附去除NO实验研究[J].化工新型材料, 2015, (7): 111-113.

    ZHANG Bo-wen, TANG Xiao-long, YI Hong-hong, ZHAO Shun-zheng, ZUO Yan-ran, WANG Zhi-xiang, GAO Feng-yu. Study on NO adsorptive removal on modified activated carbon[J]. New Chem Mater, 2015, (7): 111-113.
    [22] 张鹏宇, 杨巧云, 许绿丝, 曾汉才, 张柳.活性炭纤维低温吸附氧化NO的试验研究[J].电力科技与环保, 2004, 20(2): 25-28.

    ZHANG Peng-yu, YANG Qiao-yun, XU Lv-si, ZENG Han-cai, ZAHNG Liu. Experimental study on adsorption and oxidatiou of activated carbon fiber to NO at low temperature[J]. Electric Power Environ Protect, 2004, 20(2): 25-28.
    [23] SOUSA J P S, PEREIRA M F R, FIGUEIREDO J L. Catalytic oxidation of NO to NO2 on N-doped activated carbons[J]. Catal Today, 2011, 176(1): 383-387.
    [24] JEGUIRIM M, TSCHAMBER V, BRILHAC J F, EHRBURGER P. Interaction mechanism of NO2 with carbon black: Effect of surface oxygen complexes[J]. J Anal Appl Pyrolysis, 2004, 72(1): 171-181.
    [25] 卢静静.苯甲酸改性活性炭对燃煤烟气中元素汞的吸附机理研究[D].福建: 厦门大学, 2015.

    LU Jing-jing. Study on removal of elemental mercury from coal-fired flue gas by benzoic acid-modified activated carbon[J]. Fujian: Xiamen University, 2015.
    [26] 李兵.粉末活性炭循环流化床吸附脱除烟气中SO2的实验研究[D].山东: 山东大学, 2012.

    LI Bing. Experimental study on the adsorption removal of SO2 from flue gas by powder activated carbon in circulating fluidized bed[J]. Shandong: Shandong University, 2012.
    [27] GUO Z, XIE Y, HONG I, KIM J. Catalytic oxidation of NO to NO2 on activated carbon[J]. Energ Convers Manage, 2001, 42(15): 2005-2018.
    [28] ZHANG P, SUN H W, YU L, SUN T H. Adsorption and catalytic hydrolysis of carbaryl and atrazine on pig manure-derived biochars: impact of structural properties of biochars[J]. J Hazard Mater, 2013, 244-245(3): 217-224.
    [29] CHEN B L, JOHNSON E J, BENNY C, ZHU L Z, XING B S. Sorption of polar and nonpolar aromatic organic contaminants by plant cuticular materials: role of polarity and accessibility[J]. Environ Sci Technol, 2005, 39(16): 6138-6146.
    [30] 苏青青, 杨嘉谟.活性炭固定床吸附SO2的机理及动力学研究[J].三峡大学学报(自然科学版), 2010, 32(5): 97-101.

    SU Qing-qing, YANG Jia-mo. Mechanism and kinetic characteristics of adsorbing sulfur dioxide by activated carbon on fixed bed[J]. J Chin Three Gorges Univ (Nat Sci), 2010, 32(5): 97-101.
    [31] GUO Y, LI Y, ZHU T, YE M. Effects of concentration and adsorption product on the adsorption of SO2 and NO on activated carbon[J]. Energy Fuels, 2013, 27(1): 360-366.
    [32] 李雪飞.改性活性炭脱除烟气中NOx研究[D].北京: 煤炭科学研究总院, 2006.

    LI Xue-fei. Reduction of NOx from flue gas with modified activated carbon[J]. Beijing: China Coal Research Institute, 2006.
    [33] JIA F R, LI Z, WANG E G, HE J C, DONG H, LIU G X, JIAN W W. Preparation and SO2 adsorption behavior of coconut shell-based activated carbon via microwave-assisted oxidant activation[J]. China Pet Process Petrochen Technol, 2018, 20(1): 67-74.
    [34] 华坚, 刘宁, 尹华强, 汪南方.脱硫对活性碳表面结构的影响[J].四川大学学报(工程科学版), 2007, 39(1): 98-103.

    HUA Jian, LIU Ning, YI Hua-qiang, WANG Nan-fang. Influence of desulfuration on the surface structure of activated carbon[J]. J Chin Coal Soc, 2007, 39(1): 98-103.
  • 加载中
图(10) / 表(4)
计量
  • 文章访问数:  12
  • HTML全文浏览量:  2
  • PDF下载量:  3
  • 被引次数: 0
出版历程
  • 收稿日期:  2020-09-30
  • 修回日期:  2020-10-29
  • 刊出日期:  2020-12-10

目录

    /

    返回文章
    返回