工业原料制备大孔拟薄水铝石及在异佛尔酮选择性加氢中的应用  

Preparation of Pseudo-boehamite from Industrial Materials and Its Application in Selective Hydrogenation of Isophorone

作　　者：林锦 王芳珠[1] 吕灵灵 LIN Jin;WANG Fang-Zhu;LYU Ling-Ling(College of Chemistry and Chemical Engineering,China University of Petroleum(East China),Qingdao 266580,China)

机构地区：[1]中国石油大学(华东)化学化工学院,青岛266580

出　　处：《应用化学》2023年第1期79-90,共12页Chinese Journal of Applied Chemistry

摘　　要：以废催化裂化催化剂处理生产的工业级硫酸铝与偏铝酸钠为原料制备拟薄水铝石,探究制备工艺、扩孔和改性等对拟薄水铝石晶型、孔结构、表面酸性以及形貌的影响。用自制的拟薄水铝石经过挤条、焙烧等过程制备相应的催化剂载体,负载Pd活性组分,研究改性Al_(2)O_(3)载体以及PdCl_(2)和Pd(acac)2前驱体制备的Pd/Al_(2)O_(3)催化剂对异佛尔酮C==C选择性加氢反应的活性与选择性。通过优化反应条件得到了比表面积为413 m^(2)/g,孔容为0.84 cm^(3)/g,孔径为6.84 nm的拟薄水铝石。加入扩孔剂碳酸铵和硅酸钠后,拟薄水铝石的孔容分别增大至0.98和1.53 cm^(3)/g,平均孔径分别增至7.70和12.34 nm。以碳酸铵扩孔得到的Al_(2)O_(3)为载体和以PdCl_(2)为前驱体制备得到的Pd/Al_(2)O_(3)催化剂对异佛尔酮C==C选择性加氢活性高,达到98.69%,3,3,5-三甲基环己酮选择性>99%,活性稳定性高。Pseudo-boehmite is prepared from industrial grade aluminum sulfate and sodium meta-aluminate coming from waste FCC catalysts.The effects of preparation technology,conditions and modification on crystal type,pore structure,surface acidity and morphology of pseudo-boehmites are investigated.The activity and selectivity of Pd/Al_(2)O_(3)catalyst prepared by modified Al_(2)O_(3)carrier and PdCl_(2)and Pd(acac)2 precursors for the selective hydrogenation of isoporone C==C are studied.The pseudo-boehmite with specific surface area of 413 m^(2)/g,pore volume of 0.84 cm^(3)/g and pore size of 6.84 nm is obtained at the optimized preparation conditions.After the addition of ammonium carbonate and sodium silicate,the pore volume of pseudo-boehmite increases to 0.98 cm^(3)/g and 1.53 cm^(3)/g,and the average pore size increases to 7.70 nm and 12.34 nm,respectively.The Pd/Al_(2)O_(3)catalyst that is prepared using Al_(2)O_(3)obtained by ammonium carbonate modifier as the carrier and PdCl_(2)as the precursor shows an activity of 98.69%for the selective hydrogenation of isophorone C==C,more than 99%selectivity of 3,3,5-trimethyl-cycloheeanon(TMCH),and high activity stability.

关 键 词：拟薄水铝石 制备 改性 异佛尔酮 选择性加氢 

分 类 号：O643.3[理学—物理化学]