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新颖的PW11O39Fe(Ⅲ)(H2O)4-/H2O2类光-Fenton体系光催化降解苯胺

华英杰,王崇太*,孙振范,刘艳玲,周昌盛   

  1. (海南师范大学化学与化工学院 海口 571158)
  • 收稿日期:2011-02-08 修回日期:2011-03-17 出版日期:2012-01-10 发布日期:2012-01-10
  • 通讯作者: 王崇太，教授; Tel:0898-65736636; E-mail:wct581@sina.com; 研究方向：光、电催化及其在能源、环境领域的应用
  • 基金资助:
    国家自然科学基金(20963003)海南省重点科技项目(080305,090803)海南省自然科学基金(509009)和吉林省科技发展计划项目(20090595)资助项目

Photocatalytic Degradation of Aniline by a Novel Photo-Fenton-Like System Consisting of PW11O39Fe(Ⅲ)(H2O)4-/H2O2

HUA Yingjie, WANG Chongtai*, SUN Zhenfan, LIU Yanling, ZHOU Changsheng   

  1. (School of Chemistry and Chemical Engineering,Hainan Normal University,Haikou 571158)
  • Received:2011-02-08 Revised:2011-03-17 Published:2012-01-10 Online:2012-01-10
  • Contact: hua yingjie

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摘要：

将Keggin型铁取代杂多阴离子PW11O39Fe(Ⅲ)(H2O)4-[PW11Fe(Ⅲ)(H2O)]构成的类光-芬顿体系用于水体生物难降解有机污染物苯胺(ArNH2)的降解。 研究了在紫外光照射和H2O2存在下，PW11Fe(Ⅲ)(H2O)对ArNH2降解的均相光催化作用。 考察了ArNH2、H2O2和PW11Fe(Ⅲ)(H2O)浓度对光催化降解反应速率的影响。 实验结果表明，0.1 mmol/L PW11Fe(Ⅲ)(H2O)+0.2 mmol/L H2O2+0.1 mmol/L ArNH2的中性溶液在300 W汞灯照射下反应60 min，ArNH2的降解率达100%，总有机碳(TOC)去除约52%。 同时讨论了PW11Fe(Ⅲ)(H2O)光催化H2O2产生羟基自由基的分子机制，并比较了酸性和中性条件下苯胺的光催化降解效果。

关键词: 铁取代杂多阴离子, 均相光催化, 苯胺降解, 过氧化氢

Abstract:

A novel photo-Fenton-like system consisting of PW11O39Fe(Ⅲ)(H2O)4-[PW11Fe(Ⅲ)(H2O)] was applied to degrade the aqueous bio-refractory organic pollutant aniline(ArNH2). The homogeneous photo-catalysis of PW11Fe(Ⅲ)(H2O) for ArNH2 degradation was studied in detail under an artificial UV irradiation in the presence of hydrogen peroxide(H2O2), in which the effects of initial ArNH2, H2O2 and PW11Fe(Ⅲ)(H2O) concentration on the photo-catalytic rate of ArNH2 degradation were examined. The experimental results show that a complete ArNH2 degradation was obtained in less than 60 min in a pH=6.86 mixed phosphate solution containing 0.1 mmol/L PW11Fe(Ⅲ)(H2O)+0.2 mmol/L H2O2+0.1 mmol/L ArNH2 under a 300 W Hg lamp irradiation, and a total organic carbon(TOC) removal of ca. 52% was achieved. A mechanism of photocatalytic decomposition of H2O2 to hydroxyl radicals by PW11Fe(Ⅲ)(H2O) was proposed and a comparison of ArNH2 photo-catalytic degradation in acidic and neutral solutions was discussed.

Key words: Iron-substituted heteropolyanion, Homogeneous photocatalysis, Aniline degradation, Hydrogen peroxide

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