Ag/SBA-15低温气相选择性催化氧化苯甲醇合成苯甲醛

催化学报 , 2014, 35(1): 108-119. doi: 10.1016/S1872-2067(12)60720-7

Ag/SBA-15低温气相选择性催化氧化苯甲醇合成苯甲醛

1.齐齐哈尔大学黑龙江省普通高校精细化工重点实验室,黑龙江齐齐哈尔161006

2.齐齐哈尔大学黑龙江省普通高校精细化工重点实验室,黑龙江齐齐哈尔161006

3.齐齐哈尔大学化学与化学工程学院,黑龙江齐齐哈尔161006

4.齐齐哈尔大学化学与化学工程学院,黑龙江齐齐哈尔161006

基金项目: the Science Research Project of the Ministry of Education of Heilongjiang Province of China(12521594,2012TD012,JX201205) the National Natural Science Foundation of China(21176125) the Key Program of Science and Technology of Qiqihar,Heilongjiang Province(GYGG-201108) 齐齐哈尔市科技局项目(GYGG-201108) the Natural Science Foundation of Heilongjiang Province of China(B201114,B201313) 黑龙江省教育厅科研项目(12521594,2012TD012,JX201205) 国家自然科学基金(21176125)

关键词：银 , SBA-15 , 低温气相氧化 , 苯甲醇 , 苯甲醛

Catalytic activity of Ag/SBA-15 for low-temperature gas-phase selective oxidation of benzyl alcohol to benzaldehyde

Liang Ma ^1, , lihua Jia ^2, , Xiangfeng Guo ^3, , Lijun Xiang ^4,

1.齐齐哈尔大学黑龙江省普通高校精细化工重点实验室,黑龙江齐齐哈尔161006

2.齐齐哈尔大学黑龙江省普通高校精细化工重点实验室,黑龙江齐齐哈尔161006

3.齐齐哈尔大学化学与化学工程学院,黑龙江齐齐哈尔161006

4.齐齐哈尔大学化学与化学工程学院,黑龙江齐齐哈尔161006

Keywords： Silver , SBA-15 , Low-temperature gas-phase oxidation , Benzyl alcohol , Benzaldehyde

以SBA-15为载体,采用浸渍法制备了不同Ag含量的Ag/SBA-15,通过N2吸附-脱附、X射线衍射、扫描电子显微镜、高分辨透射电子显微镜、X射线光电子能谱和电感耦合等离子体质谱对催化剂进行了表征.将Ag/SBA-15用于苯甲醇气相选择性催化氧化合成苯甲醛,研究了反应条件对转化率和选择性的影响.结果表明,Ag/SBA-15具有均一的一维孔道结构、较厚的孔壁(3-5 nm)及较大的比表面积(411-541 m2/g),其规整纳米空间的限域作用使一定负载量的Ag以纳米尺寸均匀分散于介孔SBA-15孔道内,增加了活性组分的比表面积.亲核性氧物种从Ag到SBA-15表面的氧溢流,提高了低温下Ag/SBA-15对苯甲醇气相选择性氧化合成苯甲醛的催化性能.5.3％Ag/SBA-15中的Ag粒径为5-5 nm,且均匀分散于载体孔道中,反应温度为220℃时,苯甲醇转化率为87％,苯甲醛选择性为95％; 240℃时,苯甲醇转化率和苯甲醛选择性分别高达94％和97％;并在240-300℃范围内,其催化活性和选择性保持不变,表现出了良好的温度耐受能力.催化剂经活化再生可以连续使用40 h,选择性基本保持不变.

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