Citation: MA Xiao-ying, ZHAO Yi, XU Pei-yao, MA Shuang-chen. Removal of elemental mercury in flue gas with PMS solution catalyzed by Co doped BiFeO₃[J]. Journal of Fuel Chemistry and Technology, ;2018, 46(3): 375-384. shu

Removal of elemental mercury in flue gas with PMS solution catalyzed by Co doped BiFeO₃

School of Environmental Science and Engineering, North China Electric Power University, Baoding 071003, China

Corresponding author: MA Xiao-ying, ncepuyxm@163.com
Received Date: 11 September 2017
Revised Date: 11 January 2018

Fund Project: National Science-Technology Support Plan of China 2014BAC23B04-06Beijing Major Scientific and Technological Achievement Transformation Project of China Z151100002815012The project was supported by Fundamental Research Funds for the Central Universities 2014ZD41The project was supported by Fundamental Research Funds for the Central Universities (2014ZD41), National Science-Technology Support Plan of China (2014BAC23B04-06) and Beijing Major Scientific and Technological Achievement Transformation Project of China (Z151100002815012)

Figures(13)

A aseries of Co-doped BiFeO₃ magnetic catalysts(BiFe_1-xCo_xO₃, x=5%-20%) were synthesized by the tartaric acid sol-gel method, and the prepared catalysts were characterized using X-ray powder diffraction (XRD), Brunauer Emmett Teller (BET) technique, vibration sample magnetometer (VSM) and X ray photoelectron spectroscopy(XPS). The catalytic activity of Co doped BiFeO₃ to activate Peroxymonosulfate (PMS) was evaluated at a self-designed bubbling reactor. The effects of Co ration in catalyst, dosage of the catalyst, PMS concentration, and solution pH and reaction temperature on the removal of elemental mercury were investigated systematically, and the optimum conditions were obtained. The result indicates that the average removal efficiency of elemental mercury reaches 89.36% within 100 min under the following condition:70℃, 10% doping Co, 3.9 mmol/L PMS concentration, 0.5 g/L catalyst dosage and pH 8. Moreover, it is testified that SO₄^·- and·OH are the active species when Hg⁰ is oxidized to Hg²⁺, where the tert-butyl alcohol and ethyl alcohol are used as quenchers. Finally, the mechanisms of mercury removal with PMS solution catalyzed by BiFe_0.9Co_0.1O₃ are speculated on the basis of XPS results.
- peroxymonosulfate,
- Co doped BiFeO₃,
- sulfate radical,
- mercury
1. [1]
  ZHAO Y, HAO R L, GUO Q. A novel pre-oxidation method for elemental mercury removal utilizing a complex vaporized absorbent[J]. J Hazard Mater, 2014,280:118-126. doi: 10.1016/j.jhazmat.2014.07.061
2. [2]
  LIU Y X, WANG Y, WANG Q, PAN J F, ZHANG Y, ZHOU J, ZHANG J. A study on removal of elemental mercury in flue gas using Fenton solution[J]. J Hazard Mater, 2015,292:164-172. doi: 10.1016/j.jhazmat.2015.03.027
3. [3]
  LIU Y X, ZHOU J F, ZHANG Y C, PAN J F, WANG Q, ZHANG J. Removal of Hg⁰ and simultaneous removal of Hg⁰/SO₂/NO in flue gas using two Fenton-like reagents in a spray reactor[J]. Fuel, 2015,145:180-188. doi: 10.1016/j.fuel.2014.12.084
4. [4]
  ZHOU C, SUN L, ZHANG A, WU X, MA C, SU S. Fe_3-x Cu_xO₄ as highly active heterogeneous Fenton-like catalysts toward elemental mercury removal[J]. Chemosphere, 2015,125:16-24. doi: 10.1016/j.chemosphere.2014.12.082
5. [5]
  ZHOU C, WANG B, MA C, SONG Z J, ZENG Z. Gaseous elemental mercury removal through heterogeneous Fenton-like processes using novel magnetically separable Cu_0.3Fe_2.7-_xTi_xO₄catalysts[J]. Fuel, 2015,161(2):254-261.
6. [6]
  JI Y, KONG D, LU J, HAO J, KANG F, YIN X. Cobalt catalyzed peroxymonosulfate oxidation of tetrabromobisphenol A:Kinetics, reaction pathways, and formation of brominated by-products[J]. J Hazard Mater, 2016,313:229-237. doi: 10.1016/j.jhazmat.2016.04.033
7. [7]
  WANG Y, ZHOU L, DUAN X, SUN H, TIN EL, JIN W. Photochemical degradation of phenol solutions on Co₃O₄nanorods with sulfate radicals[J]. Catal Today, 2015,258:576-584. doi: 10.1016/j.cattod.2014.12.020
8. [8]
  DENG J, SHAO Y, GAO N, TAN C, ZHAO S, HU X. CoFe₂O₄ magnetic nanoparticles as a highly active heterogeneous catalyst of oxone for the degradation of diclofenac in water[J]. J Hazard Mater, 2013,262:836-844. doi: 10.1016/j.jhazmat.2013.09.049
9. [9]
  FENG Y, LIU J, WU D, ZHOU Z, DENG Y, ZHANG T. Efficient degradation of sulfamethazine with CuCo₂O₄ spinel nanocatalysts for peroxymonosulfate activation[J]. Chem Eng J, 2015,280:514-524. doi: 10.1016/j.cej.2015.05.121
10. [10]
  JAAFARZADEG N, GHANBARI F, AHMADI M. Catalytic degradation of 2, 4-dichlorophenoxyacetic acid (2, 4-D) by nano-Fe₂O₃ activated peroxymonosulfate:Influential factors and mechanism determination[J]. Chemosphere, 2016,169:568-576.
11. [11]
  AN J, ZHU L, WANG N, SONG Z, YANG Z, DU D, TANG H. Photo-Fenton-like degradation of tetrabromobisphenol A with graphene BiFeO₃ composite as a catalyst[J]. Chem Eng J, 2013,219:225-237. doi: 10.1016/j.cej.2013.01.013
12. [12]
  GU Y H, ZHAO J G, ZHANG W Y, LIU S, GE S P, CHEN W P, ZHANG Y. Improved ferromagnetism and ferroelectricity of La and Co co-doped BiFeO₃ ceramics with Fe vacancies[J]. Ceram Int, 2016,42(7):8863-8868. doi: 10.1016/j.ceramint.2016.02.134
13. [13]
  ZHANG L, YANG X, HAN E, ZHAO L, LIAN J. Reduced graphene oxide wrapped Fe₃O₄-Co₃O₄ yolk-shell nanostructures for advanced catalytic oxidation based on sulfate radicals[J]. Appl Surf Sci, 2017,396:945-954. doi: 10.1016/j.apsusc.2016.11.066
14. [14]
  KHARISOV B I, DIAS H V R, KHARISSOVA O V. Mini-review:Ferrite nanoparticles in the catalysis[J]. Arab J Chem, 2014:1-13.
15. [15]
  REN Y, LIN L, MA J, YANG J, FENG J, FAN Z. Sulfate radicals induced from peroxymonosulfate by magnetic ferrospinel MFe₂O₄, (M=Co, Cu, Mn, and Zn) as heterogeneous catalysts in the water[J]. Appl Catal B:Environ, 2015,165:572-578. doi: 10.1016/j.apcatb.2014.10.051
16. [16]
  CAI C, ZHANG H, ZHONG X, HOU L. Ultrasound enhanced heterogeneous activation of peroxymonosulfate by a bimetallic Fe-Co/SBA-15 catalyst for the degradation of orange Ⅱ in water[J]. J Hazard Mater, 2014,283:70-75.
17. [17]
  MADHAVAN J, MARUTHAMUTHU P, MURUGESAN S, ANANDAN S. Kinetic studies on visible light-assisted degradation of acid red 88 in presence of metal-ion coupled oxone reagent[J]. Appl Catal B:Environ, 2008,83(1/2):8-14.
18. [18]
  XU L, WANG J. Magnetic nanoscaled Fe₃O₄/CeO₂ composite as an efficient Fenton-like heterogeneous catalyst for degradation of 4-chlorophenol[J]. Environ Sci Technol, 2016,46(18):10145-10153.
19. [19]
  YU Z, WANG W, SONG L, LU L, WANG Z, JIANQ X, DONG C, QIU R. Acceleration comparison between Fe²⁺/H₂O₂, and Co²⁺/oxone for decolouration of azo dyes in homogeneous systems[J]. Chem Eng J, 2013,234:475-483. doi: 10.1016/j.cej.2013.08.013
20. [20]
  XU X, YE Q, TANG T, WANG D. Hg⁰ oxidative absorption by K₂S₂O₈solution catalyzed by Ag⁺ and Cu²⁺[J]. J Hazard Mater, 2008,158(2/3):410-416.
21. [21]
  NIKSA S, HELBLE J J, FUJIWARA N. Kinetic modeling of homogeneous mercury oxidation:The importance of NO and H₂O in predicting oxidation in coal-derived systems[J]. Environ Sci Technol, 2001,35(18):3701-3706. doi: 10.1021/es010728v
22. [22]
  GUAN Y H, MA J, REN Y M, LIU Y L, LIN LQ, ZHANG C. Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals[J]. Water Res, 2013,47(14):5431-5438. doi: 10.1016/j.watres.2013.06.023
23. [23]
  ZOU J, MA J, CHEN L, LI X, GUAN Y, XIE P, PAN C. Rapid acceleration of ferrousiron/peroxymonosulfate oxidation of organic pollutants by promoting Fe(Ⅲ)/Fe(Ⅱ) cycle with hydroxylamine[J]. Environ Sci Technol, 2013,47(20):11685-11691. doi: 10.1021/es4019145
24. [24]
  ZHANG T, ZHU H, CROUE J P. Production of sulfate radical from peroxymonosulfate induced by a magnetically separable CuFe₂O₄ spinel in water:efficiency, stability, and mechanism[J]. Environ Sci Technol, 2013,47(6):2784-2791. doi: 10.1021/es304721g
25. [25]
  WU Q, ZHANG H, ZHOU L, BAO C, ZHU H, ZHANG Y. Synthesis and application of rGO/CoFe₂O₄ composite for catalytic degradation of methylene blue on heterogeneous Fenton-like oxidation[J]. J Taiwan Inst Chem Eng, 2016,67:484-494. doi: 10.1016/j.jtice.2016.08.004
26. [26]
  XU Y, AI J, ZHANG H. The mechanism of degradation of bisphenol A using the magnetically separable CuFe₂O₄/peroxymonosulfate heterogeneous oxidation process[J]. J Hazard Mater, 2016,309:87-96. doi: 10.1016/j.jhazmat.2016.01.023
27. [27]
  HU P, LONG M. Cobalt-catalyzed sulfate radical-based advanced oxidation:A review on heterogeneous catalysts and applications[J]. Appl Catal B:Environ, 2016,181:103-117. doi: 10.1016/j.apcatb.2015.07.024
28. [28]
  TAN C, GAO N, DENG Y, DENG J, ZHOU S, LI J, XIN X. Radical induced degradation of acetaminophen with Fe₃O₄ magnetic nanoparticles as heterogeneous activator of peroxymonosulfate[J]. J Hazard Mater, 2014,276:452-460. doi: 10.1016/j.jhazmat.2014.05.068
29. [29]
  ERIC G H, SUDIPTA S, WILLIAM T S. Fenton-like reaction catalyzed by the rare earth Inner transition metal cerium[J]. Environ Sci Technol, 2008,42(13):5014-5019. doi: 10.1021/es8001508
30. [30]
  ZHAO Y, HAO R, ZHANG P, ZHOU S. An integrative process for Hg⁰ removal using vaporized H₂O₂/Na₂S₂O₈[J]. Fuel, 2014,136:113-121. doi: 10.1016/j.fuel.2014.07.046
31. [31]
  SOMMAR J, KATARINA D, STROMBERG D, FENG X. A kinetic study of the gas-phase reaction between the hydroxyl radical and atomic mercury[J]. Atmos Environ, 2001,35:3049-3054. doi: 10.1016/S1352-2310(01)00108-X
1. [1]
  Zijian Zhao , Yanxin Shi , Shicheng Li , Wenhong Ruan , Fang Zhu , Jijun Jiang . A New Exploration of the Preparation of Polyacrylic Acid by Free Radical Polymerization Based on the Concept of Green Chemistry. University Chemistry, 2024, 39(5): 315-324. doi: 10.3866/PKU.DXHX202311094
2. [2]
  Xinxin YU , Yongxing LIU , Xiaohong YI , Miao CHANG , Fei WANG , Peng WANG , Chongchen WANG . Photocatalytic peroxydisulfate activation for degrading organic pollutants over the zero-valent iron recovered from subway tunnels. Chinese Journal of Inorganic Chemistry, 2025, 41(5): 864-876. doi: 10.11862/CJIC.20240438
3. [3]
  Yuan GAO , Yiming LIU , Chunhui WANG , Zhe HAN , Chaoyue FAN , Jie QIU . A hexanuclear cerium oxo cluster stabilized by furoate: Synthesis, structure, and remarkable ability to scavenge hydroxyl radicals. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 491-498. doi: 10.11862/CJIC.20240271
4. [4]
  Lei Shi . Nucleophilicity and Electrophilicity of Radicals. University Chemistry, 2024, 39(11): 131-135. doi: 10.3866/PKU.DXHX202402018
5. [5]
  Min LIU , Huapeng RUAN , Zhongtao FENG , Xue DONG , Haiyan CUI , Xinping WANG . Neutral boron-containing radical dimers. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 123-130. doi: 10.11862/CJIC.20240362
6. [6]
  Xinhao Yan , Guoliang Hu , Ruixi Chen , Hongyu Liu , Qizhi Yao , Jiao Li , Lingling Li . Polyethylene Glycol-Ammonium Sulfate-Nitroso R Salt System for the Separation of Cobalt (II). University Chemistry, 2024, 39(6): 287-294. doi: 10.3866/PKU.DXHX202310073
7. [7]
  Jiajia Li , Xiangyu Zhang , Zhihan Yuan , Zhengyang Qian , Jian Zhu . 3D Printing Based on Photo-Induced Reversible Addition-Fragmentation Chain Transfer Polymerization. University Chemistry, 2024, 39(5): 11-19. doi: 10.3866/PKU.DXHX202309073
8. [8]
  .
  CCS Chemistry | 超分子活化底物为自由基促进高效选择性光催化氧化
  . CCS Chemistry, 2025, 7(10.31635/ccschem.025.202405229): -.
9. [9]
  Pingping LU , Shuguang ZHANG , Peipei ZHANG , Aiyun NI . Preparation of zinc sulfate open frameworks based probe materials and detection of Pb²⁺ and Fe³⁺ ions. Chinese Journal of Inorganic Chemistry, 2025, 41(5): 959-968. doi: 10.11862/CJIC.20240411
10. [10]
  Zhongyan Cao , Shengnan Jin , Yuxia Wang , Yiyi Chen , Xianqiang Kong , Yuanqing Xu . Advances in Highly Selective Reactions Involving Phenol Derivatives as Aryl Radical Precursors. University Chemistry, 2025, 40(4): 245-252. doi: 10.12461/PKU.DXHX202405186
11. [11]
  Danqing Wu , Jiajun Liu , Tianyu Li , Dazhen Xu , Zhiwei Miao . Research Progress on the Simultaneous Construction of C—O and C—X Bonds via 1,2-Difunctionalization of Olefins through Radical Pathways. University Chemistry, 2024, 39(11): 146-157. doi: 10.12461/PKU.DXHX202403087
12. [12]
  Baitong Wei , Jinxin Guo , Xigong Liu , Rongxiu Zhu , Lei Liu . Theoretical Study on the Structure, Stability of Hydrocarbon Free Radicals and Selectivity of Alkane Chlorination Reaction. University Chemistry, 2025, 40(3): 402-407. doi: 10.12461/PKU.DXHX202406003
13. [13]
  Qiuping Liu , Yongxian Fan , Wenxian Chen , Mengdi Wang , Mei Mei , Genrong Qiang . Design of Ideological and Political Education for the Preparation Experiment of Ferrous Sulfate. University Chemistry, 2024, 39(2): 116-120. doi: 10.3866/PKU.DXHX202309083
14. [14]
  Lina Feng , Guoyu Jiang , Xiaoxia Jian , Jianguo Wang . Application of Organic Radical Materials in Biomedicine. University Chemistry, 2025, 40(4): 253-260. doi: 10.12461/PKU.DXHX202405171
15. [15]
  Qiangqiang SUN , Pengcheng ZHAO , Ruoyu WU , Baoyue CAO . Multistage microporous bifunctional catalyst constructed by P-doped nickel-based sulfide ultra-thin nanosheets for energy-efficient hydrogen production from water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1151-1161. doi: 10.11862/CJIC.20230454
16. [16]
  Qin Hu , Liuyun Chen , Xinling Xie , Zuzeng Qin , Hongbing Ji , Tongming Su . Ni掺杂构建电子桥及激活MoS₂惰性基面增强光催化分解水产氢. Acta Physico-Chimica Sinica, 2024, 40(11): 2406024-. doi: 10.3866/PKU.WHXB202406024
17. [17]
  Jihua Deng , Xinshi Wu , Dichang Zhong . Exploration of Green Teaching and Ideological and Political Education in Chemical Experiment of “Preparation of Ammonium Ferrous Sulfate”. University Chemistry, 2024, 39(10): 325-329. doi: 10.12461/PKU.DXHX202405046
18. [18]
  Yuanyin Cui , Jinfeng Zhang , Hailiang Chu , Lixian Sun , Kai Dai . Rational Design of Bismuth Based Photocatalysts for Solar Energy Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2405016-. doi: 10.3866/PKU.WHXB202405016
19. [19]
  Guang Huang , Lei Li , Dingyi Zhang , Xingze Wang , Yugai Huang , Wenhui Liang , Zhifen Guo , Wenmei Jiao . Cobalt’s Valor, Nickel’s Foe: A Comprehensive Chemical Experiment Utilizing a Cobalt-based Imidazolate Framework for Nickel Ion Removal. University Chemistry, 2024, 39(8): 174-183. doi: 10.3866/PKU.DXHX202311051
20. [20]
  Jianjun LI , Mingjie REN , Lili ZHANG , Lingling ZENG , Huiling WANG , Xiangwu MENG . UV-assisted degradation of tetracycline hydrochloride by MnFe₂O₄@activated carbon activated persulfate. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1869-1880. doi: 10.11862/CJIC.20240187

Get Citation

PDF

XML

Metrics

PDF Downloads(15)
Abstract views(3080)
HTML views(1379)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Removal of elemental mercury in flue gas with PMS solution catalyzed by Co doped BiFeO3

Metrics

通讯作者: 陈斌, bchen63@163.com

Removal of elemental mercury in flue gas with PMS solution catalyzed by Co doped BiFeO₃