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作 者:张寅[1] 邵芸[1] 陈欢[1] 万海勤[1] 万玉秋[1] 郑寿荣[1]
机构地区:[1]南京大学环境学院污染控制与资源化研究国家重点实验室,南京210046
出 处:《环境科学》2012年第1期88-93,共6页Environmental Science
基 金:教育部新世纪优秀人才支持计划项目(NECT-08-0277)
摘 要:分别采用沉淀-沉积法和浸渍法合成了Pd/TiO2催化剂,采用透射电镜(TEM)、X射线衍射(XRD)和电感耦合等离子体发射光谱(ICP-AES)对材料进行了表征,并对2,4-二氯酚的催化加氢脱氯反应进行了研究.结果表明,2种方法制备的催化剂在加氢脱氯反应中均具有较好的效果,沉淀-沉积法制备的催化剂活性更高,当反应物初始浓度为3.11 mmol.L-1,pH为12,催化剂用量为50 mg时,45 min内2,4-二氯酚可以完成脱氯过程.酸性条件有利于反应的进行.当催化剂用量在15~80 mg时,反应初活性没有明显变化,因此催化反应过程不受传质阻力的影响.当反应物初始浓度在0.62~3.11 mmol.L-1时反应初活性随浓度的提高显著增加,但进一步增加反应物的浓度时初活性没有明显提高,因此2,4-二氯酚在催化剂上的加氢脱氯行为符合Langmuir-Hinshelwood模型,表明2,4-二氯酚的加氢脱氯受表面吸附所控制.Pd/TiO2 catalysts were prepared by the deposition-precipitation and impregnation methods, and were further characterized by TEM, XRD and ICP-AES. The liquid catalytic hydrodechlorination of 2,4-dichlorophenol over the catalysts was investigated. It is demonstrated that despite catalyst prepared by deposition-precipitation method exhibits higher activity than that synthesized from impregnation method, both catalysts show good performance in hydrodechlorination process. When initial concentration of the reactant was 3.11 mmol·L-1, pH was 12 and amount of catalyst used was 50 mg, hydrodechlorination of 2,4-dichlorophenol was completed within 45 min. Acidic condition facilitates hydrodechlorination process. The initial activity was not significantly influenced when the amount of catalyst used varied between 15-80 mg, which proves that mass transport limitation exerts little impact on hydrodechlorination reaction. Finally, the initial activity sharply enhanced with the increase of initial concentration of 2,4-dichlorophenol when the concentration was in the range of 0.62-3.11 mmol·L-1 while it almost remained constant with further increasing the initial concentration. Therefore, the catalytic hydrodechlorination of 2,4-dichlorophenol over Pd/TiO2-DP follows the Langumuir-Hinshelwood model, indicating that the catalytic hydrodechlorination is controlled by 2,4-dichlorophenol adsorption.
关 键 词:Pd/TiO2 2 4-二氯酚 加氢脱氯 沉淀-沉积法 浸渍法 Langmuir—Hinshelwood模型
分 类 号:X131.2[环境科学与工程—环境科学]
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