Y2O3掺杂ZrO2对苯选择加氢制环己烯催化剂Ru-La-B/ZrO2性能的影响

应用化学, 2014, 31(11): 1317-1322. doi: 10.3724/SP.J.1095.2014.40022

Y2O3掺杂ZrO2对苯选择加氢制环己烯催化剂Ru-La-B/ZrO2性能的影响

孙海杰 ^1, , 陈凌霞 ^2, , 李帅辉 ^3, , 张元馨 ^4, , 刘寿长 ^5, , 刘仲毅 ^6, , 任保增 ^7,

1.郑州大学化学与分子工程学院郑州450001;郑州师范学院化学系环境与催化工程研究所郑州450044

2.郑州师范学院化学系环境与催化工程研究所郑州450044

3.郑州大学化学与分子工程学院郑州450001

4.郑州大学化学与分子工程学院郑州450001

5.郑州大学化学与分子工程学院郑州450001

6.郑州大学化学与分子工程学院郑州450001

7.郑州大学化工与能源学院郑州450001

基金项目: the National Natural Science Foundation of China(21273205,U1304204) 河南省博士后科研项目资助(2013006) the Innovation Found for Technology Based Firms of China(10C26214104505) 国家自然科学基金资助项目(21273205,U1304204) Henan Postdoctoral Science Foundation(2013006) 国家科技型中小企业创新基金(10C26214104505)

关键词：苯 , 选择加氢 , 环己烯 , 二氧化锆 , 氧化钇掺杂

Effect of Y2O3-Doped ZrO2 on the Catalytic Performance of Ru-La-B/ZrO2 for Selective Hydrogenation of Benzene to Cyclohexene

Keywords： benzene , selective hydrogenation , cyclohexene , ZrO2 , Y2O3 doping

用水热合成法制备了纳米ZrO2和Y2O3掺杂的ZrO2(ZrO2-Y),并考察了它们作载体对苯选择加氢制环己烯催化剂Ru-La-B/ZrO2性能的影响.结果表明,2种ZrO2具有相同微晶尺寸、织构性质和粒度分布.但ZrO2仅含有单斜相ZrO2,而ZrO2-Y不但含有单斜相ZrO2,还含有一部分四方相ZrO2.Y2O3掺杂影响ZrO2的组成和物相,进而影响用其制备催化剂的组成和物相.掺杂的Y2O3可以占据一部分不适宜苯加氢生成环己烯的活性位.因此,ZrO2-Y负载Ru-La-B催化剂活性明显低于ZrO2负载的,在低苯转化率下环己烯选择性前者比后者高.由于四方相ZrO2表面羟基比单斜相少,ZrO2-Y负载Ru-La-B催化剂的亲水性比ZrO2负载的差.环己烯不易从ZrO2-Y负载的催化剂表面脱附.当苯转化率高于52％时,ZrO2-Y负载的催化剂的环己烯选择性低于单斜相ZrO2负载的.ZrO2负载的Ru-La-B催化剂上20 min的环己烯收率达到了52.1％,而ZrO2-Y负载的环己烯收率仅45.2％.纳米单斜相ZrO2较适宜作苯选择加氢制环己烯Ru催化剂的载体.

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