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用于降解4-氯酚的载钯碳纳米管催化电极研究
摘要点击 1722  全文点击 1632  投稿时间:2010-11-01  修订日期:2011-01-04
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中文关键词  电化学氧化  Pd/MWNTs  催化电极  4-氯酚  优先污染物
英文关键词  electrochemical oxidation  Pd/MWNTs  catalytic cathode  4-chlorophenol  priority pollutants
作者单位
魏祥甲 北京林业大学环境科学与工程学院北京 100083 
王辉 北京林业大学环境科学与工程学院北京 100083 
卞兆勇 北京师范大学水科学研究院北京 100875 
李敏 北京林业大学环境科学与工程学院北京 100083 
孙德智 北京林业大学环境科学与工程学院北京 100083 
中文摘要
      采用不同体积分数的硝酸溶液(8%、15%、20%、68%)对多壁碳纳米管(MWNTs)进行预处理,使用甲醛还原方法制备出Pd/MWNTs催化剂,利用Boehm滴定法、红外光谱分析、X射线衍射(XRD)、扫描电子显微镜(SEM)及循环伏安曲线(CV)对催化剂进行表征分析,并制备成Pd/MWNTs催化阴极,在隔膜电解体系中对4-氯酚进行降解研究.结果表明,随着硝酸体积分数的增加,预处理后碳纳米管表面酸性基团的数量呈上升趋势,经过68%硝酸预处理2 h后,酸性基团的量达到2.3 mmol/g,羧基数量达到0.38 mmol/g.制得的Pd/MWNTs催化剂上金属Pd粒径大小为9.2 nm,高度分散在碳纳米管表面; 在碳纳米管上负载金属Pd可以促进H2O2的生成,同时做为电极使用时可以减小外加电压,降低能耗.Pd/MWNTs催化电极对4-氯酚有较好的降解效果,在前80 min通氢气条件下,阴极室发生还原性脱氯反应,后60 min通入空气,阴阳极室发生了氧化反应,4-氯酚转化率和TOC去除率分别达到86.9%和71.6%。
英文摘要
      Nitric acid in various volume fraction(8%, 15%, 20%, and 68%) was used on the multi-wall carbon nanotubes(MWNTs) pre-treatment and then the formaldehyde reduction method was utilized for the preparation the Pd/MWNTs catalysts which were fully characterized by Boehm titration method, X-ray diffraction(XRD), infrared spectroscopy, scanning electron microscopy(SEM), and cyclic voltammetry(CV) techniques. The electrochemical degradation of 4-chlorophenol was investigated in a diaphragm electrolysis system using the Pd/MWNTs gas-diffusion cathode. The results indicated that the active organic function groups increased on the surface of the carbon nanotube pre-treated by using 68% nitric acid. Pd particles with an average size of 9.2 nm were highly dispersed in the carbon nanotube with an amorphous structure. Additionally, the Pd/MWNTs catalyst in Pd/MWNTs gas-diffusion electrode system accelerated the two-electron reduction of O2 to hydrogen peroxide(H2O2) when feeding air. The Pd/MWNTs gas-diffusion cathode can not only reductively dechlorinate 4-chlorophenols by feeding hydrogen gas, but also accelerate the two-electron reduction of O2 to H2O2 by feeding air. Therefore, the removal efficiency and the average removal efficiency of 4-chlorophenol in terms of total organic carbon(TOC) reached about 86.9% and 71.6% after 140 min electrolysis, respectively.

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