Cuo和CeO_2在氯化氢氧化反应中的协同作用  

Synergetic Effects of CuO and CeO_2 on Hydrogen Chloride Catalytic Oxidation

作　　者：曹锐[1] 费兆阳[1,2] 陈献[1] 汤吉海[1] 崔咪芬[1] 乔旭[1,2] 

机构地区：[1]南京工业大学化学化工学院 [2]南京工业大学材料化学工程国家重点实验室,江苏南京210009

出　　处：《化学反应工程与工艺》2013年第4期295-300,共6页Chemical Reaction Engineering and Technology

基　　金：国家科技支撑计划(2011BAE18B01);江苏省基础研究计划(自然科学基金)重点项目(BK2010083);江苏省科技支撑计划(BE2011830)

摘　　要：以Y分子筛为载体,采用浸渍法制备了CuO/Y、CeO_2/Y和CuO-CeO_2/Y催化剂用于氯化氢氧化制氯反应,并采用扫描电镜(SEM)、X-射线衍射(XRD)、比表面积测试法(BET)、拉曼光谱分析法(Raman)和H_2-程序升温还原法(H_2-TPR)等多种手段表征了催化剂特性,对反应前后的催化剂进行SEM、XRD以及BET表征,结果显示催化剂具有良好的结构稳定性。CuO和CeO_2的氯化氢氧化反应特性研究表明,CuO在反应气氛中会被氯化,氯化铜物种聚集导致CuO/Y比表面积下降;CeO_2未被氯化且在载体表面更加分散。催化性能考察结果显示,CuO-CeO_2/Y催化剂在390℃下对HC1的转化率达到90%,其性能明显优于CeO_2/Y和CuO/Y催化剂,说明CuO与CeO_2存在显著的协同效应。Raman光谱表明铜离子进入CeO_2体相使其发生了晶格畸变,H_2-TPR结果表明CeO_2能够提高CuO的分散度,改善其氧化还原性能。CeO_2促进铜物种的分散并使得分散铜物种量的增多是CuO-CeO_2/Y催化剂性能提升的主要原因。CuO/Y, CeO2/Y and CuO-CeO2/Y catalysts for hydrogen chloride oxidation were prepared by impregnation method. The catalysts were characterized by means of scanning electron microscope （SEM）, X-ray diffraction（XRD）, Brurauer Emmerr Teller Procedure（BET）, Raman and temperature programmed reduction（H2-TPR）. The results of SEM, XRD and BET showed that the structure of the catalysts kept stable during the reaction. CuO and CeO2 displayed different reaction character： CuO was chlorinated, and the aggregation of the chlorinated copper species resulted in the decreasing of surface area of CuO/Y-U; while CeO2 did not undergo chlorinated and become more disperse. The results of the catalytic performance test showed that CuO-CeO2/Y catalyst exhibited the highest activity, and the conversion of HC1 was 90% at 390 ℃, indicating the significant synergetic effects between CuO and CeO2. The results of Raman and H2-TPR showed that cupric ion entered into CeO2 lattice, leading to the lattice deformation. On the other hand, CeO2 could improve the dispersion and redox property of CuO. Over the CuO-CeOEfY catalyst, the high dispersion of copper species was responsible for the high catalytic performance.

关 键 词：氧化铜 氧化铈 氯化氢氧化 协同作用 

分 类 号：TQ624.82[化学工程—精细化工]