邹冲,戴 勇,费兆阳,陈献,汤吉海,崔咪芬,乔旭.限域纳米空间制备高效HCl氧化CuO-CeO2催化剂[J].分子催化,2015,(3):238-245 |
限域纳米空间制备高效HCl氧化CuO-CeO2催化剂 |
Synthesis of efficient CuO-CeO2 catalysts in limited nanospace for HCl oxidation |
投稿时间:2015-04-23 修订日期:2015-06-11 |
DOI: |
中文关键词: CuO-CeO2 硬模板 氯化氢 氯气 氧空位 |
英文关键词:CuO-CeO2 hard template HCl chloride oxygen vacancies |
基金项目:国家科技支撑计划(2011BAE18B01); 国家自然科学青年基金(21306089); 江苏省高校自然科学基金面上项目(13KJB530006) |
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中文摘要: |
利用KIT-6的有序介孔作为限域空间制备了一系列的介孔CuO-CeO2催化剂。借助XRD、BET、Raman、ESEM、TEM和H2-TPR等手段对催化剂进行表征,并考察其在HCl氧化反应中的催化性能。结果表明:铜含量<35%时,CuO物种高度分散在催化剂的表面或者进入CeO2晶格,催化剂具有高比表面积(>140m2.g-1)和较小的晶粒尺寸,其中25CuO-CeO2催化剂具备最高的表面氧空位浓度和最优的低温氧化还原性能,并在HCl氧化反应中表现出最佳的催化活性,O2/HCl=6,370 °C时转化率达到90%。反应动力学结果表明, 25CuO-CeO2中更多的高分散的CuO促进了HCl在催化剂表面的吸附和活化,更高浓度的氧空位增强了氧分子的吸附和活化。 |
英文摘要: |
A series of meosoporous CuO-CeO2 composite catalysts were prepared using the ordered pores of hard template KIT-6 as a limited nanospace. The prepared catalysts were characterized by XRD, BET, Raman, ESEM , TEM and H2-TPR.The performance of catalysts for gas-phase HCl catalytic oxidation to Cl2 were also investigated. The results showed that CuO species could highly disperse on the surface of CuO-CeO2 catalysts with Cu loading below 35%, as well as some Cu2+ dissolved into the CeO2 lattice. In addition, the catalysts gained good surface area (>140m2.g-1) and small grain size. Among all catalysts, 25CuO-CeO2 obtained the highest surface oxygen vacancies concentrations, suitable CuO dispersion and best reducibility at low temperature, leading to a 90% conversion of HCl at 370 oC (O2/HCl=6). Kinetic studies showed that the more highly dispersed CuO provided more active sites for HCl adsorption and activation, while the oxgen vacancies could obviously enhanced the adsorption and activation of gas-phase oxygen. |
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