高级搜索

Ce-MCM-41分子筛用于臭氧氧化对氯苯甲酸的活性评价

,  ,  ,  ,  ,  , 

downloadPDF

上一篇

下一篇

邴吉帅, 曾俊喻, 廖高祖, 李旭凯, 蓝冰燕, 张秋云, 李来胜. Ce-MCM-41分子筛用于臭氧氧化对氯苯甲酸的活性评价[J]. 环境化学, 2012, 31(5): 653-657.
引用本文: 邴吉帅, 曾俊喻, 廖高祖, 李旭凯, 蓝冰燕, 张秋云, 李来胜. Ce-MCM-41分子筛用于臭氧氧化对氯苯甲酸的活性评价[J]. 环境化学, 2012, 31(5): 653-657.
shu
BING Jishuai, ZENG Junyu, LIAO Gaozu, LI Xukai, LAN Bingyan, ZHANG Qiuyun, LI Laisheng. Synthesis of cerium-doped MCM-41 for ozonation of p-chlorobenzoic acid[J]. Environmental Chemistry, 2012, 31(5): 653-657.
Citation: BING Jishuai, ZENG Junyu, LIAO Gaozu, LI Xukai, LAN Bingyan, ZHANG Qiuyun, LI Laisheng. Synthesis of cerium-doped MCM-41 for ozonation of p-chlorobenzoic acid[J]. Environmental Chemistry, 2012, 31(5): 653-657.
shu

Ce-MCM-41分子筛用于臭氧氧化对氯苯甲酸的活性评价

  • 1.

    华南师范大学化学与环境学院, 广州, 510006

  • 基金项目:

    国家自然科学基金(20977036)资助.

Synthesis of cerium-doped MCM-41 for ozonation of p-chlorobenzoic acid

  • 1.

    School of Chemistry & Environment, South China Normal University, Guangzhou, 510006, China

  • Fund Project:

  • 摘要: 通过水热法合成了铈掺杂MCM-41(Ce-MCM-41)介孔分子筛,并将其用于臭氧氧化水中对氯苯甲酸(p-CBA).小角X射线衍射(XRD)、氮气吸附-脱附(BET)、紫外可见漫反射光谱(UV-Vis DRS)、透射电镜(TEM)表征结果表明,铈成功进入MCM-41分子筛骨架,以正四面体形式存在,且Ce-MCM-41保持了纯硅MCM-41有序的介孔结构,具有较高的比表面积;铈的掺杂显著提高MCM-41催化臭氧氧化对氯苯甲酸的活性,反应60 min后,TOC去除率由MCM-41的63%提高到86% (Si/Ce = 60),而单独臭氧氧化仅为52%;铈的溶出仅为0.085 mg·L-1,较同样负载量的铈负载Ce/MCM-41的溶出(0.44 mg·L-1)有较大减少.催化剂重复使用3次后仍保持较高的活性,这表明Ce-MCM-41具有较好的活性和稳定性,是一种有前景的臭氧氧化催化剂.
    Abstract: Cerium-doped MCM-41 (Ce-MCM-41) was prepared by a hydrothermal method and its catalytic activity for ozonation of p-chlorobenzoic acid (p-CBA) in aqueous solution was studied. Ce-MCM-41 was characterized by low angle X-ray powder diffraction (XRD), nitrogen adsorption-desorption(BET), ultraviolet-visible diffuse reflection spectrum (UV-Vis DRS) and transmission electron microscopy (TEM). The results showed that the material retained a highly ordered mesopore structure of pure silica MCM-41 and had a high surface area. Cerium was incorporated into the framework of MCM-41, locating at tetrahedrally coordinated sites. Ce-MCM-41 significantly improved the effect of ozone oxidation. After 60 min reaction time, TOC removal rate was 63% with MCM-41, 86% with Ce-MCM-41 (Si/Ce=60), while only 52% with O3 alone. Besides, Ce-MCM-41 had much less cerium leaching (0.085 mg稬-1) compared with that of Ce/MCM-41 (0.44 mg稬-1). After being used for three times, TOC removal rate decreased only by 5%, while p-CBA removal rate kept nearly constant. Ce-MCM-41 is a promising catalyst for ozonation process.
  • 加载中
  • [1] Kresge C T, Leonowicz M E, Roth W J, et al. Ordered mesoporous molecular sieves synthesized by a liquid-crystal template mechanism[J]. Nature,1992,359:710-712
    [2] Zhang A J, Li Z H, Li Z C, et al. Effects of different Ti-doping methods on the structure of pure-silica MCM-41 mesoporous materials[J]. Applied Surface Science, 2008, 254:6298-6304
    [3] Kong Y, Jiang S Y, Wang J, et al. Synthesis and characterization of Cu-Ti-MCM41[J]. Microporous and Mesoporous Materials, 2005, 86: 191-197
    [4] Wang G J, Wang Y R, Liu Y W, et al. Synthesis of highly regular mesoporous Al-MCM-41 from metakaolin[J]. Applied Clay Science, 2009, 44:185-188
    [5] Parida K M, Dash Suresh K. Adsorption of Cu2+ on spherical Fe-MCM-41 and its application for oxidation of adamantine[J]. Journal of Hazardous Materials, 2010, 179:642-649
    [6] Eswaramoorthi I, Sundaramurthy V, Lingappan N. Hydroisomerisation of C6-C7 n-alkanes over Pt loaded zirconium containing Al-MCM-41 molecular sieves[J]. Microporous and Mesoporous Materials, 2004, 71:109-115
    [7] Pîrvulescu V, Anastasescu C, Su B L. Bimetallic Ru-(Cr, Ni, or Cu) and La-(Co or Mn) incorporated MCM-41 molecular sieves as catalysts for oxidation of aromatic hydrocarbons[J]. Journal of Molecular Catalysis A: Chemical, 2004, 211:143-148
    [8] Vinu A, Nandhini K.U. Murugesan V, et al. Mesoporous FeAlMCM-41: an improved catalyst for the vapor phase tert-butylation of phenol[J]. Applied Catalysis A: General, 2004, 265:1-10
    [9] Zhan W C, Guo Y L, Wang Y Q, et al. Synthesis of lanthanum-doped MCM-48 molecular sieves and its catalytic performance for the oxidation of styrene[J]. Journal of Physical Chemistry B, 2007, 111:12103-12110
    [10] Ma J, Qin Q D, Liu K. Adsorption of nitrobenzene from aqueous solution by MCM-41[J]. Journal of Colloid and Interface Science, 2007, 315:80-86
    [11] Sepehrian H, Fasihi J, Khayatzadeh Mahani M. Adsorption behavior studies of picric acid on mesoporous MCM-41[J]. Industrial & Engineering Chemistry Research, 2009, 48:6772-6775
    [12] Benhamou A, Baudu M, Derriche Z, et al. Aqueous heavy metals removal on amine-functionalized Si-MCM-41 and Si-MCM-48[J]. Journal of Hazardous Materials, 2009, 171:1001-1008
    [13] Sui M H, Liu J, Sheng L. Mesoporous material supported manganese oxides (MnO<em>x/MCM-41) catalytic ozonation of nitrobenzene in water[J]. Applied Catalysis B: Environmental, 2011, 106:195-203
    [14] Zhao Q, Xu Y H, Li Y H, et al. Effect of the Si/Ce molar ratio on the textural properties of rare earth element cerium incorporated mesoporous molecular sieves obtained room temperature[J]. Applied Surface Science, 2009, 255:9425-9429
    [15] Boutros M, Launay F, Nowicki A, et al. Reduced forms of Rh(Ⅲ) containing MCM-41 silicas as hydrogenation catalysts for arene derivatives[J]. Journal of Molecular Catalysis A: Chemical, 2006, 259:91-98
    [16] Zhan W C, Lu G Z, Guo Y L, et al. Synthesis of Ln-doped MCM-41 mesoporous materials and their catalytic performance in oxidation of styrene[J]. Journal of Rare Earths, 2008, 26:59-65
    [17] Dai Q G, Wang X Y, Chen G P, et al. Direct synthesis of cerium(Ⅲ)-incorporated SBA-15 mesoporous molecular sieves by two-step synthesis method[J]. Microporous and Mesoporous Materials, 2007, 100:268-275
    [18] 王幸宜,催化剂表征[M]. 上海:华东理工大学出版社,2008:169-177
  • 加载中
WeChat 点击查看大图
计量
  • 文章访问数:  753
  • HTML全文浏览数:  688
  • PDF下载数:  674
  • 施引文献:  0
出版历程
  • 收稿日期:  2011-09-21

Ce-MCM-41分子筛用于臭氧氧化对氯苯甲酸的活性评价

  • 1. 华南师范大学化学与环境学院, 广州, 510006
  • 收稿日期:  2011-09-21
基金项目:

国家自然科学基金(20977036)资助.

摘要: 通过水热法合成了铈掺杂MCM-41(Ce-MCM-41)介孔分子筛,并将其用于臭氧氧化水中对氯苯甲酸(p-CBA).小角X射线衍射(XRD)、氮气吸附-脱附(BET)、紫外可见漫反射光谱(UV-Vis DRS)、透射电镜(TEM)表征结果表明,铈成功进入MCM-41分子筛骨架,以正四面体形式存在,且Ce-MCM-41保持了纯硅MCM-41有序的介孔结构,具有较高的比表面积;铈的掺杂显著提高MCM-41催化臭氧氧化对氯苯甲酸的活性,反应60 min后,TOC去除率由MCM-41的63%提高到86% (Si/Ce = 60),而单独臭氧氧化仅为52%;铈的溶出仅为0.085 mg·L-1,较同样负载量的铈负载Ce/MCM-41的溶出(0.44 mg·L-1)有较大减少.催化剂重复使用3次后仍保持较高的活性,这表明Ce-MCM-41具有较好的活性和稳定性,是一种有前景的臭氧氧化催化剂.

English Abstract

    全文HTML

参考文献 (18)

目录

/

返回文章
返回

Copyright © 2019 中国科学院生态环境研究中心