Citation: SHI Qi-qi, WANG Yu-ting, SHEN Bo-xiong, ZHANG Xiao. Synthesis of hierarchical porous carbon loaded with chlorine and its mercury removal performance[J]. Journal of Fuel Chemistry and Technology, ;2019, 47(8): 1000-1007. shu

Synthesis of hierarchical porous carbon loaded with chlorine and its mercury removal performance

SHI Qi-qi ¹ ,
WANG Yu-ting ¹ ,
SHEN Bo-xiong ^1,2,, ,
ZHANG Xiao ^1,2,,

1.
School of Energy and Environment Engineering, Hebei University of Technology, Tianjin 300401, China;
2.
Tianjin Key Laboratory of Clean Energy and Pollution Control, Tianjin 300401, China

Corresponding author: SHEN Bo-xiong, shenbx@hebut.edu.cn ZHANG Xiao, zhangxiao@hebut.edu.cn
Received Date: 12 March 2019
Revised Date: 12 May 2019

Fund Project: Tangshan Science and Technology Project 18130211ATianjin Science Popularization Project 18KPXMSF00080Tianjin Natural Science Foundation Key Project 18JCZDJC39800the National Natural Science Foundation Youth Project 51808181The project was supported by the National Natural Science Foundation Youth Project (51808181), Tianjin Natural Science Foundation Key Project (18JCZDJC39800), Tianjin Science and Technology Major Special Project and Engineering (18ZXSZSF00040), Tianjin Science Popularization Project (18KPXMSF00080), Tianjin Platform Project (18PTZWHZ00010) and Tangshan Science and Technology Project (18130211A)Tianjin Platform Project 18PTZWHZ00010Tianjin Science and Technology Major Special Project and Engineering 18ZXSZSF00040

Figures(7)

Chlorine-loaded hierarchical porous bio-char was prepared by co-pyrolysis using nano-CaCO₃ as template and rice straw as carbon precursor. The removal of mercury (Hg⁰) from flue gas by porous materials was studied on a fixed bed test bench with simulated flue gas. The materials were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), N₂ adsorption-desorption (BET), temperature programmed desorption (Hg-TPD) and X-ray photoelectron spectroscopy (XPS). The results show that HCl impregnation not only removes the products on the template to form porous structures but also effectively loads chlorine onto the surface of the material. The specific surface area and total pore volume of B1C1-Cl2 are 398.1 m²/g and 0.4923 cm³/g, respectively. When the GHSV is 225000 h^-1 at 120 ℃, the removal efficiency of Hg⁰ by chemical adsorption is up to 95%. The porous structure is beneficial to gas diffusion and the high specific surface area can provide more active sites. The covalent groups (C-Cl) participating in the Hg⁰ removal process are the dominant chemical adsorption sites on the inner micro-mesopore surface.
- elemental mercury,
- porous bio-chars,
- chlorine,
- adsorption,
- flue gas
1. [1]
  GAO Lan-jun, WANG Fu-mei, WU Han-ming, PAN Yi-jun, SHEN Bo-xiong. Synthesis of mesoprous materials with Ce-Co/KIT-6 and its mercury removal performance[J]. J Fuel Chem Technol, 2017,45(8):1017-1024. doi: 10.3969/j.issn.0253-2409.2017.08.016
2. [2]
  ZHOU Q, DUAN Y F, CHEN M M, LIU M, LU P. Studies on mercury adsorption species and equilibrium on activated carbon surface[J]. Energy Fuels, 2017,31(12):14211-14218. doi: 10.1021/acs.energyfuels.7b02699
3. [3]
  LI H L, WU C Y, LI Y, ZHANG J Y. Superior activity of MnO_x-CeO₂/TiO₂ catalyst for catalytic oxidation of elemental mercury at low flue gas temperatures[J]. Appl Catal B:Environ, 2012,111/112:381-388. doi: 10.1016/j.apcatb.2011.10.021
4. [4]
  XU Y, ZENG X B, LUO G Q, ZHANG B, XU P, XU M H, YAO H. Chlorine-char composite synthesized by co-pyrolysis of biomass wastes and polyvinyl chloride for elemental mercury removal[J]. Fuel, 2016,183:73-79. doi: 10.1016/j.fuel.2016.06.024
5. [5]
  LI G L, WANG S X, WANG F M, WU Q R, TANG Y, SHEN B X. Role of inherent active constituents on mercury adsorption capacity of chars from four solid wastes[J]. Chem Eng J, 2017,307:544-552. doi: 10.1016/j.cej.2016.08.106
6. [6]
  WU J, LI Z, SONG Y. Preparation of biomass-derived hierarchically porous carbon/Co₃O₄ nanocomposites as anode materials for lithium-ion batteries[J]. J Alloy Compd, 2016,656:745-752. doi: 10.1016/j.jallcom.2015.10.063
7. [7]
  XU B, HOU S S, ZHANG F, ZHANG F L, CAO G P, CHU M, YANG Y S. Nitrogen-doped mesoporous carbon derived from biopolymer as electrode material for supercapacitors[J]. J Electroanal Chem, 2014,712:146-150. doi: 10.1016/j.jelechem.2013.11.020
8. [8]
  ISLAM M A, TAN I A W, BENHOURIA A, BEN A, ASIF M, HAMEED B H. Mesoporous and adsorptive properties of palm date seed activated carbon prepared via sequential hydrothermal carbonization and sodium hydroxide activation[J]. Chem Eng J, 2015,270:187-195. doi: 10.1016/j.cej.2015.01.058
9. [9]
  ZHAO P F, GUO X, ZHENG C G. Removal of elemental mercury by iodine-modified rice husk ash sorbents[J]. J Environ Sci-China, 2010,22(10):1629-1636. doi: 10.1016/S1001-0742(09)60299-0
10. [10]
  XU B, PENG L, WANG G, CAO G P, WU F. Easy synthesis of mesoporous carbon using nano-CaCO₃ as template[J]. Carbon, 2010,48(8):2377-2380. doi: 10.1016/j.carbon.2010.03.003
11. [11]
  CAO B, LIU H, XU B, LEI Y F, CHEN X H, SONG H H. Mesoporous soft carbon as an anode material for sodium ion batteries with superior rate and cycling performance[J]. J Mater Chem A, 2016,4(17):6472-6478. doi: 10.1039/C6TA00950F
12. [12]
  LI G L, SHEN B X, LI Y W, ZHAO B, WANG F M, HE C, WANG Y Y, ZHANG M. Removal of element mercury by medicine residue derived biochars in presence of various gas compositions[J]. J Hazard Mater, 2015,298:162-169. doi: 10.1016/j.jhazmat.2015.05.031
13. [13]
  ZU G Q, SHEN J, ZOU L O, WANG F, WANG X D, ZHANG Y W, YAO X D. Nanocellulose-derived highly porous carbon aerogels for supercapacitors[J]. Carbon, 2015,99:203-211.
14. [14]
  KONG L J, LIU M X, DIAO Z H, CHEN D Y, CHANG X Y, XIONG Y. Coupling template nanocasting and self-activation for fabrication of nanoporous carbon[J]. Sci Rep, 2016,638176. doi: 10.1038/srep38176
15. [15]
  WANG T, WU J W, ZHANG Y S, LIU J, SUI Z F, ZHANG H C, CHEN W Y, NORRIS P, PAN W P. Increasing the chlorine active sites in the micropores of biochar for improved mercury adsorption[J]. Fuel, 2018,229:60-67. doi: 10.1016/j.fuel.2018.05.028
16. [16]
  GHORISHI S B, KEENEY R M, SERRE S D. Development of a Cl-impregnated activated carbon for entrained-flow capture of elemental mercury[J]. Environ Sci Technol, 2002,36(20):4454-4459. doi: 10.1021/es0255608
17. [17]
  LI G L, WANG S X, WU Q R, WANG F Y, SHEN B X. Mercury sorption study of halides modified bio-chars derived from cotton straw[J]. Chem Eng J, 2016,302:305-313. doi: 10.1016/j.cej.2016.05.045
18. [18]
  IRIARTE-VELASCO U, SIERRA I, ZUDAIRE L, AYASTUY J L. Preparation of a porous biochar from the acid activation of pork bones[J]. Food Bioprod Process, 2016,98:341-353. doi: 10.1016/j.fbp.2016.03.003
19. [19]
  LI G L, WANG S X, WU Q G, WA NG, F Y, DING D, SHEN B X. Mechanism identification of temperature influence on mercury adsorption capacity of different halides modified bio-chars[J]. Chem Eng J, 2017,315:251-261. doi: 10.1016/j.cej.2017.01.030
20. [20]
  LI G L, SHEN B X, WANG Y, YUE S J, XI Y Q, AN M D, REN K K. Comparative study of element mercury removal by three bio-chars from various solid wastes[J]. Fuel, 2015,145:189-195. doi: 10.1016/j.fuel.2014.12.083
21. [21]
  SANO A, TAKAOKA M, SHIOTA K. Vapor-phase elemental mercury adsorption by activated carbon co-impregnated with sulfur and chlorine[J]. Chem Eng J, 2017,315:598-607. doi: 10.1016/j.cej.2017.01.035
22. [22]
  LEE S F, SEO Y C, JURNG J, LEE T G. Removal of gas-phase elemental mercury by iodine- and chlorine-impregnated activated carbons[J]. Atmos Environ, 2004,38(29):4887-4893. doi: 10.1016/j.atmosenv.2004.05.043
23. [23]
  XU Y, ZENG X B, ZHANG B, ZHU X Q, ZHOU M L, ZOU R J, SUN P, LUO G Q, YAO H. Experiment and kinetic study of elemental mercury adsorption over a novel chlorinated sorbent derived from coal and waste polyvinyl chloride[J]. Energy Fuels, 2016,30(12):10635-10642. doi: 10.1021/acs.energyfuels.6b01372
24. [24]
  XU Y, LUO G Q, HE S W, DENG F F, PANG Q, XU Y Q, YAO H. Efficient removal of elemental mercury by magnetic chlorinated biochars derived from co-pyrolysis of Fe(NO₃)₃-laden wood and polyvinyl chloride waste[J]. Fuel, 2019,239:982-990. doi: 10.1016/j.fuel.2018.11.102
25. [25]
  ZHAO Peng-fei, GUO Xin, ZHENG Chu-guang. Investigating the mechanism of elemental mercury binding on activated carbon and chlorine-embedded activated carbon[J]. Proc CSEE, 2010,30(23):40-44.
1. [1]
  Yutao Lu , Jing Wu . Rebirth from the Flames: Unveiling the “Chemical Secrets” of Fire Smoke. University Chemistry, 2024, 39(9): 208-213. doi: 10.12461/PKU.DXHX202401001
2. [2]
  Jingke LIU , Jia CHEN , Yingchao HAN . Nano hydroxyapatite stable suspension system: Preparation and cobalt adsorption performance. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1763-1774. doi: 10.11862/CJIC.20240060
3. [3]
  Hui Wang , Abdelkader Labidi , Menghan Ren , Feroz Shaik , Chuanyi Wang . Recent Progress of Microstructure-Regulated g-C₃N₄ in Photocatalytic NO Conversion: The Pivotal Roles of Adsorption/Activation Sites. Acta Physico-Chimica Sinica, 2025, 41(5): 100039-0. doi: 10.1016/j.actphy.2024.100039
4. [4]
  Peng XU , Shasha WANG , Nannan CHEN , Ao WANG , Dongmei YU . Preparation of three-layer magnetic composite Fe₃O₄@polyacrylic acid@ZiF-8 for efficient removal of malachite green in water. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 544-554. doi: 10.11862/CJIC.20230239
5. [5]
  Zeyu XU , Anlei DANG , Bihua DENG , Xiaoxin ZUO , Yu LU , Ping YANG , Wenzhu YIN . Evaluation of the efficacy of graphene oxide quantum dots as an ovalbumin delivery platform and adjuvant for immune enhancement. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1065-1078. doi: 10.11862/CJIC.20240099
6. [6]
  Jing Wang , Pingping Li , Yuehui Wang , Yifan Xiu , Bingqian Zhang , Shuwen Wang , Hongtao Gao . Treatment and Discharge Evaluation of Phosphorus-Containing Wastewater. University Chemistry, 2024, 39(5): 52-62. doi: 10.3866/PKU.DXHX202309097
7. [7]
  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
8. [8]
  Fugui XI , Du LI , Zhourui YAN , Hui WANG , Junyu XIANG , Zhiyun DONG . Functionalized zirconium metal-organic frameworks for the removal of tetracycline from water. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 683-694. doi: 10.11862/CJIC.20240291
9. [9]
  Wei Li , Jinfan Xu , Yongjun Zhang , Ying Guan . 共价有机框架整体材料的制备及食品安全非靶向筛查应用——推荐一个仪器分析综合化学实验. University Chemistry, 2025, 40(6): 276-285. doi: 10.12461/PKU.DXHX202406013
10. [10]
  Jianan Zhang , Mengzhen Xu , Jiamin Liu , Yufei He . 面向“双碳”目标的脱氯吸附剂开发研究型综合实验设计. University Chemistry, 2025, 40(6): 248-255. doi: 10.12461/PKU.DXHX202408068
11. [11]
  Xiaosong PU , Hangkai WU , Taohong LI , Huijuan LI , Shouqing LIU , Yuanbo HUANG , Xuemei LI . Adsorption performance and removal mechanism of Cd(Ⅱ) in water by magnesium modified carbon foam. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1537-1548. doi: 10.11862/CJIC.20240030
12. [12]
  Yang ZHOU , Lili YAN , Wenjuan ZHANG , Pinhua RAO . Thermal regeneration of biogas residue biochar and the ammonia nitrogen adsorption properties. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1574-1588. doi: 10.11862/CJIC.20250032
13. [13]
  Shuanglin TIAN , Tinghong GAO , Yutao LIU , Qian CHEN , Quan XIE , Qingquan XIAO , Yongchao LIANG . First-principles study of adsorption of Cl₂ and CO gas molecules by transition metal-doped g-GaN. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1189-1200. doi: 10.11862/CJIC.20230482
14. [14]
  Qianqian ZHU , Lihui XU , Hong PAN , Chengjian YAO , Hong ZHAO , Nan MA , Xiaolin SHI , Zihan SHEN , Weijun ZHANG , Zhongjian WANG . Waste cotton fabric-ased porous carbon materials: Preparation and wave-absorbing properties. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1555-1564. doi: 10.11862/CJIC.20250040
15. [15]
  Hongting Yan , Aili Feng , Rongxiu Zhu , Lei Liu , Dongju Zhang . Reexamination of the Iodine-Catalyzed Chlorination Reaction of Chlorobenzene Using Computational Chemistry Methods. University Chemistry, 2025, 40(3): 16-22. doi: 10.12461/PKU.DXHX202403010
16. [16]
  Jiaqi AN , Yunle LIU , Jianxuan SHANG , Yan GUO , Ce LIU , Fanlong ZENG , Anyang LI , Wenyuan WANG . Reactivity of extremely bulky silylaminogermylene chloride and bonding analysis of a cubic tetragermylene. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1511-1518. doi: 10.11862/CJIC.20240072
17. [17]
  Yongpo Zhang , Xinfeng Li , Yafei Song , Mengyao Sun , Congcong Yin , Chunyan Gao , Jinzhong Zhao . Synthesis of Chlorine-Bridged Binuclear Cu(I) Complexes Based on Conjugation-Driven Cu(II) Oxidized Secondary Amines. University Chemistry, 2024, 39(5): 44-51. doi: 10.3866/PKU.DXHX202309092
18. [18]
  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
19. [19]
  Ruonan Li , Shijie Liang , Yunhua Xu , Cuifen Zhang , Zheng Tang , Baiqiao Liu , Weiwei Li . Chlorine-Substituted Double-Cable Conjugated Polymers with Near-Infrared Absorption for Low Energy Loss Single-Component Organic Solar Cells. Acta Physico-Chimica Sinica, 2024, 40(8): 2307037-0. doi: 10.3866/PKU.WHXB202307037
20. [20]
  Jizhou Liu , Chenbin Ai , Chenrui Hu , Bei Cheng , Jianjun Zhang . Accelerated Interfacial Electron Transfer in Perovskite Solar Cell by Ammonium Hexachlorostannate Modification and fs-TAS Investigation. Acta Physico-Chimica Sinica, 2024, 40(11): 2402006-0. doi: 10.3866/PKU.WHXB202402006

Get Citation

PDF

XML

Metrics

PDF Downloads(8)
Abstract views(552)
HTML views(38)

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