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SO42-/ZrO2型固体超强酸改性及其催化氧化脱除噻吩类硫化物

Modification of solid super acid catalyst SO42-/ZrO2 and its catalytic activity for oxidation reaction of thiophene

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【作者】 姬乔娜张伟余谟鑫李忠

【Author】 JI Qiao-na,ZHANG Wei,YU Mo-xin,LI Zhong(School of Chemistry and Chemical Engineering,South China University of Technology,The Key Laboratory of Enhanced Heat Transfer and Energy Conversation Ministry of Education,Guangzhou 510640,China)

【机构】 华南理工大学化学与化工学院,传热强化与过程节能教育部重点实验室

【摘要】 通过掺杂不同金属元素对SO42-/ZrO2型固体超强酸进行改性,应用共沉淀法制备了一系列固体酸催化剂SO42-/ZrO2、SO42-/ZrO2-ZnO、SO42-/ZrO2-Fe2O3、SO24-/ZrO2-CuO、SO42-/ZrO2-Al2O3,利用氧气作氧化剂进行催化氧化脱除噻吩硫化物动力学实验。研究结果表明,掺杂了Zn、Fe和Cu的SO24-/ZrO2型催化剂催化氧化效果较SO42-/ZrO2都有明显提高,其中添加了金属Zn的SO42-/ZrO2-ZnO催化氧化效果最好,在反应温度为50℃,能达到100%的脱硫率。对合成的系列固体酸进行了X射线衍射(XRD)、氨程序升温脱附(NH3-TPD)的表征,结果表明,催化剂样品中四方相ZrO2的含量越高,表面酸含量越大,其催化氧化噻吩硫化物的活性越高。

【Abstract】 The solid super acid catalyst SO2-4/ZrO2 was modified by doping with different metal oxides,and then a series of modified solid super acid catalysts such as,SO2-4/ZrO2,SO2-4/ZrO2-ZnO,SO2-4/ZrO2-Fe2O3,SO2-4/ZrO2-CuO and SO2-4/ZrO2-Al2O3 were obtained by coprecipitation method.With oxygen as oxidant,the catalytic oxidation kinetic experiments of thiophene over the modified solid super acid catalysts were carried out.Results showed that doping Zn,Fe,Cu metal oxides to SO2-4/ZrO2 can improve the catalytic oxidation activity of the catalysts,of which the catalytic activity of SO2-4/ZrO2-ZnO was the highest and the conversion efficiency of thiophene can reach 100% at 50℃.The characterization results of the catalysts by powder X-ray diffraction (XRD) and temperature programmed desorption of ammonia(NH3-TPD)showed that the more the content of T-ZrO2 on the catalyst surfaces was,the more its acid amounts was,and thus it had higher catalytic activity.

【基金】 国家自然科学基金资助项目(20806026);广东省重点基金资助项目(8251064101000018);中国博士后基金资助项目(200804-30834)
  • 【文献出处】 功能材料 ,Journal of Functional Materials , 编辑部邮箱 ,2009年11期
  • 【分类号】TE624.5;O643.36
  • 【被引频次】16
  • 【下载频次】326
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