高级搜索

煤基活性炭表面改性对稀土负载型CeO2/AC低温脱硝性能的影响

,  ,  ,  ,  ,  ,  ,  ,  , 

downloadPDF

上一篇

下一篇

陈薇, 肖高, 郭杰, 刘明华, 齐赛男, 刘学虎, 李军, 华坚, 王涛, 李新. 煤基活性炭表面改性对稀土负载型CeO2/AC低温脱硝性能的影响[J]. 环境工程学报, 2018, 12(7): 1959-1967. doi: 10.12030/j.cjee.201712188
引用本文: 陈薇, 肖高, 郭杰, 刘明华, 齐赛男, 刘学虎, 李军, 华坚, 王涛, 李新. 煤基活性炭表面改性对稀土负载型CeO2/AC低温脱硝性能的影响[J]. 环境工程学报, 2018, 12(7): 1959-1967. doi: 10.12030/j.cjee.201712188
shu
CHEN Wei, XIAO Gao, GUO Jie, LIU Minghua, QI Sainan, LIU Xuehu, LI Jun, HUA Jian, WANG Tao, LI Xin. Effect of surface modification of coal based activated carbon on low temperature denitrification performance of rare-earth supported CeO2/AC[J]. Chinese Journal of Environmental Engineering, 2018, 12(7): 1959-1967. doi: 10.12030/j.cjee.201712188
Citation: CHEN Wei, XIAO Gao, GUO Jie, LIU Minghua, QI Sainan, LIU Xuehu, LI Jun, HUA Jian, WANG Tao, LI Xin. Effect of surface modification of coal based activated carbon on low temperature denitrification performance of rare-earth supported CeO2/AC[J]. Chinese Journal of Environmental Engineering, 2018, 12(7): 1959-1967. doi: 10.12030/j.cjee.201712188
shu

煤基活性炭表面改性对稀土负载型CeO2/AC低温脱硝性能的影响

  • 1.

    福州大学环境与资源学院，福州 350108

  • 2.

    中国人民解放军军事科学院防化研究院，北京 102205

  • 3.

    四川大学轻纺与食品学院，成都 610065

  • 4.

    成都国化环保科技有限公司，成都 610065

  • 基金项目:

    国家自然科学基金资助项目（21506036）

    福建省自然科学基金资助项目（2017J01412）

    福建省教育厅中青年教师教育科研项目（JA15099，JA14062）

    中国人民解放军军事科学院防化研究院（823093）

    福州大学国家级大学生创新训练计划项目（201610386021）

Effect of surface modification of coal based activated carbon on low temperature denitrification performance of rare-earth supported CeO2/AC

  • 1.

    College of Environment and Resouces, Fuzhou University, Fuzhou 350108, China

  • 2.

    Institute of Chemical Defense, Academy of Military Science of the Chinese People’s Liberation Army, Beijing 102205, China

  • 3.

    College of Light Industry, Textile and Food Engineering, Sichuan University, Chengdu 610065, China

  • 4.

    Chengdu Guohua Environmental Protection Technology Co.Ltd., Chengdu 610065, China

  • Fund Project:

  • 摘要: 以煤基活性炭（AC）为载体，在不同温度下分别采用空气热氧化和硝酸浸渍对其进行预氧化表面改性处理，然后将稀土金属Ce3+负载在预氧化改性后的活性炭载体上，经煅烧而制得改性CeO2/AC低温SCR脱硝剂。并采用N2等温吸附脱附测试、X 射线光电子能谱等表征手段考察了2种不同预氧化改性方式对基炭孔结构和表面物化性质的影响。同时研究了不同预氧化方式、稀土负载量、煅烧温度对脱硝剂的低温脱硝性能的影响。结果表明：空气热氧化预处理的AC相对于原炭而言，比表面积没有明显损失，且基炭表面官能团得到了明显丰富；而经硝酸氧化的活性炭，比表面积有明显下降。制备CeO2/AC低温脱硝剂的最佳工艺为：在350 ℃下，采用空气热氧化预处理，稀土负载量为5% (质量分数)， 500 ℃ N2保护煅烧温度下，所得到的CeO2/AC脱硝剂具有最佳低温脱硝活性。该脱硝剂在脱硝温度为150 ℃即可达到100%的脱硝率。
    Abstract: This work presented the preparation process of modified activated carbon supported Ce3+ for SCR denitration. As the catalyst support, coal-based activated carbon was pretreated by two methods of thermal oxidation by air and wet chemical oxidation by dipping nitric acid. The pore structure and surface chemical properties of the modified activated carbon by different methods was investigated by N2 adsorption and X-ray photoelectron spectrometer (XPS). The results show that the BET surface of modified activated carbon by hot air presented no obvious loss and the surface functional groups of activated carbon was obviously enriched. However, the BET surface of modified activated carbon by dipping nitric acid showed significantly reduce. Moreover, we also discovered the optimum preparation process of Ce3+ supported modified activated carbon (CeO2/AC) as SCR denitration catalyst. When the temperature of hot air oxidation is 350 ℃, the loading amount of Ce is 5% (mass fraction) by dipping method, and the calcining temperature is 500 ℃ under the protection of nitrogen, the obtained denitration catalyst CeO2/AC has the optimum SCR catalytic activity and its denitration rate can reach 100% at 150 ℃.
  • 加载中
  • [1] LIU Y X, WANG Y, LIU Z, et al.Oxidation removal of nitric oxide from flue gas using uv photolysis of aqueous hypochlorite [J].Environmental Science & Technology,2017,51(20):11950-11959 10.1021/acs.est.7b03628
    [2] SONG X Y, MA X L, NING G Q, et al.Pitch-based nitrogen-doped mesoporous carbon for flue gas desulfurization[J].Industrial & Engineering Chemistry Research,2017,56(16):4743-4749 10.1021/acs.iecr.7b00054
    [3] REN S, GUO F Q, YANG J, et al.Selection of carbon materials and modification methods in low-temperature sintering flue gas denitrification[J].Chemical Engineering Research and Design,2017,126:278-285 10.1016/j.cherd.2017.08.022
    [4] LIU Y X, LIU Z Y, WANG Y, et al.Simultaneous absorption of SO2 and NO from flue gas using ultrasound/Fe2+/heat coactivated persulfate system[J].Journal of Hazardous Materials,2018,342:326-334 10.1016/j.jhazmat.2017.08.042
    [5] MENG D M, ZHAN W C, GUO Y, et al.A highly effective catalyst of Sm-MnOx for the NH3-SCR of NOx at low temperature: The promotional role of Sm and its catalytic performance[J].ACS Catalysis,2015,5(10):5973-5983 10.1021/acscatal.5b007
    [6] ZHAN S H, ZHANG H, ZHANG Y, et al.Efficient NH3-SCR removal of NOx with highly ordered mesoporous WO3(χ)-CeO2 at low temperatures[J].Applied Catalysis B: Environmental,2017,203:199-209 10.1016/j.apcatb.2016.10.010
    [7] SHEN M Q, LI C X, WANG J Q, et al.New insight into the promotion effect of Cu doped V2O5/WO3–TiO2 for low temperature NH3-SCR performance[J].RSC Advances,2015,5(44):35155-35165 10.1039/C5RA04940G
    [8] LIU Z M, LI Y, ZHU T L, et al.Selective catalytic reduction of NOx by NH3 over Mn-promoted V2O5/TiO2 catalyst[J].Industrial & Engineering Chemistry Research,2014,53(33):12964-12970 10.1021/ie501887f
    [9] CHI G L, SHEN B X, YU R R, et al.Simultaneous removal of NO and Hg0 over Ce-Cu modified V2O5/TiO2 based commercial SCR catalysts[J].Journal of Hazardous Materials,2017,330:83-92 10.1016/j.jhazmat.2017.02.013
    [10] DONG W L, YOO B R.Advanced metal oxide (supported) catalysts: Synthesis and applications[J].Journal of Industrial & Engineering Chemistry,2014,20(6):3947-3959 10.1016/j.jiec.2014.08.004
    [11] 石晓燕, 丁世鹏, 贺泓,等. 改进钒基SCR脱硝催化剂的抗碱金属中毒性能 [J]. 环境工程学报,2014,8(5):2031-2034
    [12] 杨超, 程华, 黄碧纯. 工业催化抗SO2和 H2O中毒的低温NH3-SCR脱硝催化剂研究进展 [J]. 化工进展,2014(4):907-913 10.3969/j.issn.1000-6613.2014.04.020
    [13] JIANG L J, LIU Q C, ZHAO Q, et al.Promotional effect of Ce on the SCR of NO with NH3, at low temperature over MnOx supported by nitric acid-modified activated carbon[J].Research on Chemical Intermediates,2017,435:1-16 10.1016/j.catcom.2010.10.028
    [14] LIU Y, NING P, LI K, et al.Simultaneous removal of NOx, and SO2, by low-temperature selective catalytic reduction over modified activated carbon catalysts[J].Russian Journal of Physical Chemistry A,2017,91(3):490-499 10.1134/S003602441703030
    [15] YOSHIKAWA M, YASUTAKE A, MOCHIDA I.Low-temperature selective catalytic reduction of NOx by metal oxides supported on active carbon fibers[J].Applied Catalysis A：General,1998,173(2):239-245 10.1016/S0926-860X(98)00182-3
    [16] 沈伯雄，郭宾彬，史展亮，等.CeO2/ACF的低温SCR烟气脱硝性能研究[J]. 燃料化学学报,2007,35(1):125-128
    [17] SHAN W P, LIU F D, YU Y B, et al.The use of ceria for the selective catalytic reduction of NOx, with NH3[J].Chinese Journal of Catalysis,2014,35(8):1251-1259 10.1016/S1872-2067(14)60155-8
    [18] YAO X J, GONG Y T, LI H L, et al.Research progress of ceria-based catalysts in the selective catalytic reduction of NOx by NH3[J].Acta Physico-Chimica Sinica,2015,31(5):817-828 10.3866/PKU.WHXB201503253
    [19] JIN Q J, SHEN Y S, ZHU S M, et al.Rare earth ions (La, Nd, Sm, Gd, and Tm) regulate the catalytic performance of CeO2/Al2O3 for NH3-SCR of NO[J].Journal of Materials Research,2017,32:1-8 10.1557/jmr.2017.125
    [20] 黄增斌, 李翠清, 王振,等. 不同分子筛负载锰铈催化剂的低温NH3-SCR脱硝性能[J]. 燃料化学学报,2016,44(11):1388-1393 10.3969/j.issn.0253-2409.2016.11.016
    [21] ZHU H, HAN W F, LIU H Z.Influence of oxidation on heat-treated activated carbon support properties and metallic dispersion of Ru/C catalyst[J].Catalysis Letters,2007,115(1/2):13-18 10.1007/s10562-007-9068-y
    [22] AUER E，FREUND A，PIETSCH J，et al.Carbons as supports for industrial precious metal catalysts[J].Applied Catalysis A: General,1998,173(2):259-271 10.1016/S0926-860X(98)00184-7
    [23] 刘秋芳, 周艳波, 王丽,等. 活性炭预处理对Pd/AC催化剂上NO吸附性能的影响[J]. 复旦学报(自然科学版),2012,51(5):678-683
    [24] 周静, 于才渊. 改性炭基催化剂低温烟气选择性还原脱硝性能研究[J]. 干燥技术与设备,2015(2):33-38
    [25] 褚有群, 韩文锋, 童少平,等. 活性炭表面性质对氧气扩散电极电催化性能的影响[J]. 催化学报,2006,27(2):183-188
    [26] 单晓梅，杜铭华，朱书全，等. 活性炭表面改性及吸附极性气体[J]. 煤炭转化,2003,26(1):32-36
    [27] QI G S, YANG R T.Performance and kinetics study for low-temperature SCR of NO with NH3 over MnOx-CeO2 catalyst[J].Journal of Catalysis,2003,217(2):434-441 10.1016/S0021-9517(03)00081-2
    [28] 吴彦霞, 房晶瑞, 雷本喜,等. 载体的制备条件对Mn-Ce/TiO2催化剂脱硝活性的影响[J]. 武汉理工大学学报,2013,35(7):37-41
    [29] 张东辉，王卓晖，宋存义，等. 改性活性炭纤维负载锰铈复合氧化物低温选择性催化还原脱硝 [J]. 北京科技大学学报,2012,34(010):1102-1107
    [30] DONG W K, HONG S C.Correlation between physicochemical properties of various commercial TiO2 supports and NH3-SCR activities of Ce/Ti catalysts [J].Journal of the Korean Industrial & Engineering Chemistry,2015,26(2):193-198 10.14478/ace.2015.1012
    [31] 张信莉, 王栋, 彭建升,等. 煅烧温度对Mn改性γ-Fe2O3催化剂结构及低温SCR脱硝活性的影响 [J]. 燃料化学学报,2015,43(02):243-250
  • 加载中
WeChat 点击查看大图
计量
  • 文章访问数:  2982
  • HTML全文浏览数:  2695
  • PDF下载数:  296
  • 施引文献:  0
出版历程
  • 刊出日期:  2018-07-26

煤基活性炭表面改性对稀土负载型CeO2/AC低温脱硝性能的影响

  • 1. 福州大学环境与资源学院，福州 350108
  • 2. 中国人民解放军军事科学院防化研究院，北京 102205
  • 3. 四川大学轻纺与食品学院，成都 610065
  • 4. 成都国化环保科技有限公司，成都 610065
基金项目:

国家自然科学基金资助项目（21506036）

福建省自然科学基金资助项目（2017J01412）

福建省教育厅中青年教师教育科研项目（JA15099，JA14062）

中国人民解放军军事科学院防化研究院（823093）

福州大学国家级大学生创新训练计划项目（201610386021）

摘要: 以煤基活性炭（AC）为载体，在不同温度下分别采用空气热氧化和硝酸浸渍对其进行预氧化表面改性处理，然后将稀土金属Ce3+负载在预氧化改性后的活性炭载体上，经煅烧而制得改性CeO2/AC低温SCR脱硝剂。并采用N2等温吸附脱附测试、X 射线光电子能谱等表征手段考察了2种不同预氧化改性方式对基炭孔结构和表面物化性质的影响。同时研究了不同预氧化方式、稀土负载量、煅烧温度对脱硝剂的低温脱硝性能的影响。结果表明：空气热氧化预处理的AC相对于原炭而言，比表面积没有明显损失，且基炭表面官能团得到了明显丰富；而经硝酸氧化的活性炭，比表面积有明显下降。制备CeO2/AC低温脱硝剂的最佳工艺为：在350 ℃下，采用空气热氧化预处理，稀土负载量为5% (质量分数)， 500 ℃ N2保护煅烧温度下，所得到的CeO2/AC脱硝剂具有最佳低温脱硝活性。该脱硝剂在脱硝温度为150 ℃即可达到100%的脱硝率。

English Abstract

参考文献 (31)

目录

/

返回文章
返回

Copyright © 2019 中国科学院生态环境研究中心