摘要
以硅藻土为载体,采用浸渍法制备出Cs_xH_(6-x)P_2 W_(18)O_(62)·nH_2O/硅藻土催化剂。对催化剂进行FT-IR、XRD、SEM、NH_3-TPD及N_2吸附-脱附表征。将该催化剂用于催化H_2O_2氧化环己酮合成己二酸,并考察了Cs离子取代度和Cs_xH_(6-x)P_2 W_(18)O_(62)·nH_2O负载量对催化活性的影响。结果表明,30%Cs_3H_3P_2W_(18)O_(62)/硅藻土的催化活性最高。采用正交设计方法得到对己二酸收率影响由大到小的因素依次为H_2O_2用量、反应时间、反应温度、催化剂用量,最佳工艺条件为催化剂用量占环己酮质量分数5.1%、n(C_6H_(10)O)/n(30%H_2O_2)=1/5、反应温度105℃、反应时间5.0h,此时己二酸的收率为85.3%,纯度为99.9%。30%Cs_3H_3P_2W_(18)O_(62)/硅藻土具有良好的稳定性,重复使用5次,己二酸收率仍可达70.1%。
CsxH6-xP2W18O62·nH2O/Diatomite catalysts were prepared by impregnation method and characterized by FT-IR, XRD, SEM, NH3-TPD and N2 adsorption-desorption techniques. The prepared catalysts were then used in the oxidation of cyclohexanone to adipic acid with Hz Oz. The effects of Cs ion exchange degree and loading amount of CsxH6-xP2W18O62·nH2O/ on the catalytic behavior of CsxH6-xP2W18O62·nH2O/Diatomite were investigated, showing that CsxH6-xP2W18O62·nH2O/Diatomite with CsxH6-xP2W18O62·nH2O loading amount of 30% exhibited the best catalytic activity. According to the influence degree from large to small, the factors affecting the yield of adipic acid were in the order of H2O2 quantity, reaction time, reaction temperature and catalyst dosage, which was the conclusion of orthogonal experiments, and the obtained optimal reaction conditions were the mass fraction of catalyst to cyclohexanone of 5.1%, n（CGH10O）/n（30%H2O2）=1/5, reaction temperature of 105℃ and reaction time of 5 h, under which the yield and purity of adipic acid were 85.3 % and 99 %, respectively. 30CsxH6-xP2W18O62·nH2O/Diatomite also showed good catalytic stability with the adipic acid yield still of 70.1 % after 5 recycle times, and was easily removed from the system after reaction.
出处
《石油学报（石油加工）》
EI
CAS
CSCD
北大核心
2015年第6期1430-1437,共8页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家自然科学基金项目(21161009)
江西省自然科学基金项目(20132BAB203004和20122BAB213001)
江西省教育厅科技项目(GJJ14731)
九江学院科技项目(2013KJ005)资助
关键词
Dawson结构磷钨酸铯
硅藻土
己二酸
催化氧化
cesium salts of Dawson-type tunstophosphoric acids
diatomite
adipic acid
catalyticoxidation
