天然水体主要本底成分对催化臭氧氧化草酸的影响
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  • 英文篇名:Effect of Background Constituents on Catalytic Ozonation of Oxalic Acid
  • 作者:李旭凯 ; 郭杏妹 ; 张秋云 ; 李来胜
  • 英文作者:LI Xukai;GUO Xingmei;ZHANG Qiuyun;LI Laisheng;School of Chemistry & Environment,South China Normal University;
  • 关键词:催化臭氧氧化 ; Fe2O3 ; 活性炭 ; 草酸 ; 本底成分
  • 英文关键词:catalytic ozonation;;Fe2O3;;activated carbons;;oxalic acid;;background constituents
  • 中文刊名:HNSF
  • 英文刊名:Journal of South China Normal University(Natural Science Edition)
  • 机构:华南师范大学化学与环境学院;
  • 出版日期:2017-04-25
  • 出版单位:华南师范大学学报(自然科学版)
  • 年:2017
  • 期:v.49
  • 基金:国家科技重大专项项目(2012ZX07206003);; 华南师范大学青年教师科研培育基金项目(14KJ07)
  • 语种:中文;
  • 页:HNSF201702015
  • 页数:5
  • CN:02
  • ISSN:44-1138/N
  • 分类号:86-90
摘要
采用浸渍法制备了Fe_2O_3负载活性炭(Fe_2O_3/AC)催化剂,考察了Fe_2O_3/AC催化臭氧氧化草酸的活性以及天然水体主要本底成分对Fe_2O_3/AC催化臭氧氧化草酸的影响.结果表明,臭氧氧化草酸过程中Fe_2O_3/AC显示了良好的催化活性,草酸的去除主要基于催化贡献.HCO_3~-、CO_3~(2-)及腐殖酸对Fe_2O_3/AC催化臭氧氧化草酸均有抑制作用.加入HCO_3~-和CO_3~(2-)使催化臭氧氧化草酸体系pH升高,进而降低Fe_2O_3/AC催化臭氧氧化草酸的活性.此外,HCO_3~-和CO_3~(2-)也是羟基自由基抑制剂,HCO_3~-、CO_3~(2-)对草酸去除的抑制作用从侧面验证了Fe_2O_3/AC催化臭氧氧化草酸遵循羟基自由基机理.腐殖酸加入体系后,与草酸形成竞争吸附和竞争氧化,从而抑制草酸的降解.
        The aim of this research was to investigate catalytic activity of Fe_2O_3 loaded activated carbon catalyst(Fe_2O_3/AC) prepared by the dipping method,and the effect of background constituents on catalytic ozonation of oxalic acid.The results indicated that Fe_2O_3/AC showed good activity in ozonation of oxalic acid,and the removal of oxalic acid was mainly based on catalytic contribution.Some background constituents such as HCO_3~-,CO_3~(2-) and humic acid could cause the inhibition of oxalic acid degradation in Fe_2O_3/AC catalytic ozonation.The addition of HCO_3~-,CO_3~(2-) increased the pH value of system,and therefore the activity of Fe_2O_3/AC decreased.The inhibition of oxalic acid degradation indirectly proved that catalytic ozonation of oxalic acid in the presence of Fe_2O_3/AC followed the mechanism of hydroxyl radical oxidation.The humic acid competed with oxalic acid to be adsorbed and oxidized which led to the inhibition of oxalic acid degradation.
引文
[1]NAWROCKI J.Catalytic ozonation in water:controversies and questions.Discussion paper[J].Applied Catalysis B:Environmental,2013,142/143(5):465-471.
    [2]LEGUBE B,LEITNER N K V.Catalytic ozonation:a promising advanced oxidation technology for water treatment[J].Catalysis Today,1999,53(1):61-72.
    [3]XING S T,LU X Y,LIU J,et al.Catalytic ozonation o sulfosalicylic acid over manganese oxide supported on mesoporous ceria[J].Chemosphere,2016,144:7-12.
    [4]叶伟莹,张秋云,刘佩红.活性炭负载铈催化臭氧氧化水中邻苯二甲酸二甲酯研究[J].华南师范大学学报(自然科学版),2009(2):79-83.YE W Y,ZHANG Q Y,LIU P H.Study on catalytic ozonation of dimethyl phthalate over cerium/activated carbon catalyst[J].Journal of South China Normal University(Natural Science Edition),2009(2):79-83.
    [5]KEYKAVOOS R,MANKIDY R,MA H,et al.Mineralization of bisphenol A by catalytic ozonation over alumina[J].Separation and Purication Technology,2013,107(4):310-317.
    [6]唐莉莉,刘杰,黄瑞欢,等.Fe/MCM-41催化臭氧氧化水中对氯苯甲酸的研究[J].华南师范大学学报(自然科学版),2013,45(2):74-78.TANG L L,LIU J,HUANG R H.Catalytic ozonation of pchlorobenzoic acid in aqueous solution by Fe/MCM-41[J].Journal of South China Normal University(Natura Science Edition),2013,45(2):74-78.
    [7]LI X K,ZHANG Q Y,TANG L L,et al.Catalytic ozonation of p-chlorobenzoic acid by activated carbon and nickel supported activated carbon prepared from petroleum coke[J].Journal of Hazardous Materials,2009,163(1):115-120.
    [8]李来胜,孙强强.用于催化臭氧氧化的金属改性MCM-41研究进展[J].华南师范大学学报(自然科学版),2013,45(6):124-128.LI L S,SUN Q Q.Advance in metal modification of mesoporous molecular sieve MCM-41 for catalytic ozonation[J].Journal of South China Normal University(Natural Science Edition),2013,45(6):124-128.
    [9]FARIA P C C,ORFAO J J M,PEREIRA M F R.Catalytic ozonation of sulfonated aromatic compounds in the presence of activated carbon[J].Applied Catalysis B:Environmental,2008,83(1/2):150-159.
    [10]SUN Q Q,WANG Y,LI L S,et al.Mechanism for enhanced degradation of clofibric acid in aqueous by catalytic ozonation over Mn Ox/SBA-15[J].Journal of Hazardous Materials,2015,286:276-284.
    [11]PETRE A L,CARBAJO J B,ROSAL R,et al.Cu O/SBA-15 catalyst for the catalytic ozonation of mesoxalic and oxalic acids.Water matrix effects[J].Chemical Engineering Journal,2013,225(3):164-173.
    [12]SUN Q Q,LI L S,YAN H H,et al.Influence of the surface hydroxyl groups of Mn Ox/SBA-15 on heterogeneous catalytic ozonation of oxalic acid[J].Chemical Engineering Journal,2014,242(8):348-356.
    [13]赵雷,马军,孙志忠,等.蜂窝陶瓷催化臭氧化降解水中痕量硝基苯的机理研究[J].环境科学,2007,28(2):335-341.ZHAO L,MA J,SUN Z Z,et al.Study on mechanism of ceramic honeycomb-catalytic ozonation for the decomposition of trace nitrobenzene in aqueous solution[J].Environmental Science,2007,28(2):335-341.
    [14]孙志忠,赵雷,马军.水中本底成分对催化臭氧化分解微量硝基苯的影响[J].环境科学,2006,27(2):285-289.SUN Z Z,ZHAO L,MA J.Effect of background constituents on the degradation of trace nitrobenzene in aqueous solution by catalytic ozonation[J].Environmental Science,2006,27(2):285-289.
    [15]周文敏,符建荣,肖华,等.水中本底成分对催化臭氧氧化降解富里酸的影响[J].农业环境科学学报,2013,32(1):191-196.ZHOU W M,FU J R,XIAO H,et al.Effect of background constituents on the degradation of fulvic acid in aqueous solution by catalytic ozonation[J].Journal of Agro-Environment Science,2013,32(1):191-196.
    [16]BELTRAN F J,RIVAS F J,FERNANDEZ L A,et al.Kinetics of catalytic ozonation of oxalic acid in water with activated carbon[J].Industrial and Engineering Chemistry Research,2002,41(25):6510-6517.
    [17]BUXTON G V,GREENSTOCK C L,HELMAN W P,et al.Critical review of rate constants for reactions of hydrated electrons,hydrogen atoms and hydroxyl radicals(·OH/·O-)in aqueous solution[J].Journal of Physical and Chemical Reference Data,1988,17(2):513-886.
    [18]HOIGNE J,BADER H.Rate constants of reactions of ozone with organic and inorganic compounds in water-I:non-dissociating organic compounds[J].Water Research,1983,17:173-183.
    [19]孙志忠,赵雷,马军.改性蜂窝陶瓷催化臭氧化降解水中微量硝基苯[J].环境科学,2005,26(6):84-88.SUN Z Z,ZHAO L,MA J.Degradation of nitrobenzene in aqueous solution by modified ceramic honeycomb-catalyzed ozonation[J].Environmental Science,2005,26(6):84-88.
    [20]MA J,GRAHAM N J D.Degradation of atrazine by manganese-catalyzed ozonation:influence of radical scavengers[J].Water Research,2000,34(15):3822-3828.
    [21]GUNTEN U V.Ozonation of drinking water:Part I.Oxidation kinetics and product formation[J].Water Research,2003,37(7):1443-1467.
    [22]STAEHELIN J,HOIGNE J.Decomposition of ozone in water:rate of initiation by hydroxide ions and hydrogen peroxide[J].Environmental Science&Technology,1982,16(10):676-681.
    [23]FARIA P C C,ORFAO J J M,PEREIRA M F R.Activated carbon catalytic ozonation of oxamic and oxalic acids[J].Applied Catalysis B:Environmental,2008,79(3):237-243.
    [24]HUANG R H,YAN H H,LI L S,et al.Catalytic activity of Fe/SBA-15 for ozonation of dimethyl phthalate in aqueous solution[J].Applied Catalysis B:Environmental,2011,106(1/2):264-271.
    [25]MA J,GRAHAM N J D.Degradation of atrazine by manganese catalysed ozonation:influence of humic substances[J].Water Research,1999,33(3):785-793.
    [26]STAEHELIN J,HOIGNJ.Decomposition of ozone in water in the presence of organic solutes acting as promoters and inhibitors of radical chain reactions[J].Environmental Science&Technology,1985,19(12):1206-1213.
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