表面含氧基团对AuCl3-CuCl2／C双组分非汞催化剂催化性能的影响  

Effect of Surface Oxygen Groups on the Two-component Non-mercury AuCl_3-CuCl_2/C Catalyst

作　　者：程晓光[1] 赵基钢[1] 王雷[1,2] 任若凡 杨恒华[2] 沈本贤[1] 

机构地区：[1]华东理工大学 化学工程联合国家重点实验室,上海200237 [2]天津大沽化工股份有限公司,天津300455

出　　处：《高等学校化学学报》2014年第3期582-588,共7页Chemical Journal of Chinese Universities

基　　金：中央高校基本科研业务费专项资金(批准号:WA1214003);天津市滨海新区塘沽科技发展专项资金(批准号:2012STHB04-01)资助~~

摘　　要：采用HNO3氧化及在He气氛围经不同温度焙烧处理椰壳活性炭,以此活性炭为载体,通过浸渍法制得AuCl3-CuCl2/C双组分非汞催化剂,并用于乙炔氢氯化反应评价.结果表明,分别以HNO3处理、未处理和400℃焙烧处理活性炭为载体的催化剂乙炔转化率最高分别可达98%,96%和90%;而以700和1000℃焙烧的活性炭为载体的催化剂反应4 h后乙炔转化率急剧下降为30%.考察了活性炭表面的含氧基团(尤其是羟基)对Au基催化剂的催化性能的影响.The coconut shell activated carbon was oxidized by HNO3 and calcined at different temperature in the atmosphere of He. It demonstrated that the physical properties of the activated carbons were basically identical before and after different treatments. However, the content of surface oxygen groups, such as phenol and carboxylic, were increased after oxidizing by HNO3 and decreased in the order of carboxyl, phenol and carbonyl after calcing in different temperatures. Taking the above activated carbons as the carrier, two-compo-nent catalysts of AuCl3-CuCl2 were prepared by impregnation method. And the catalysts were evaluated by the acetylene hydrochlorination. The results showed that the acetylene conversion rates of the catalysts, which were prepared with the carrier of original activated carbon, pre-treated by HNO3 oxidation and calcined in 400 ℃ for 1 h, could reach above 96%, 98%and 90%, respectively. And they had good reaction stability in 10 h. The acetylene conversion rates dropped sharply to around 30% after 4 h for the AuCl3-CuCl2/He700-C and AuCl3-CuCl2/He1000-C catalysts, whose carriers were calcined in 700 and 1000 ℃. The analysis results by BET, H2-TPR and SEM show that the BET specific surface area decreases mostly, carbon deposition is more serious and active component dispersion is poorer. It prove that the surface oxygen groups, especially for the hydroxyl group, plays an important role in promoting the dispersion of Au, enhancing the stability and reducing the carbon deposition.

关 键 词：乙炔氢氯化 含氧基团 分散性 稳定性 活性炭 

分 类 号：O643[理学—物理化学]