吴藏藏,郑丽,徐秀峰.Mn-Al和Cu-Mn-Al复合氧化物催化苯甲醇选择氧化反应[J].分子催化(中英文),2016,30(6):532-539 |
Mn-Al和Cu-Mn-Al复合氧化物催化苯甲醇选择氧化反应 |
Selective catalytic oxidation of benzyl alcohol over Mn-Al and Cu-Mn-Al composite oxide catalysts |
投稿时间:2016-11-16 修订日期:2016-12-20 |
DOI: |
中文关键词: 苯甲醇选择氧化 Mn-Al复合氧化物 Cu-Mn-Al复合氧化物 催化活性 苯甲醛选择性 |
英文关键词:Selective oxidation of benzyl alcohol Mn-Al composite oxides Cu-Mn-Al composite oxides Catalytic activity Selectivity of benzaldehyde |
基金项目:山东省重点研发计划项目 |
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中文摘要: |
用溶胶-凝胶法制备了不同组成的Mn-Al和Cu-Mn-Al复合氧化物,用于催化苯甲醇选择氧化制苯甲醛。用X射线衍射(XRD)、N2物理吸附(BET)、扫描电镜(SEM)、H2程序升温还原(H2-TPR)、O2程序升温脱附(O2-TPD)和X射线光电子能谱(XPS)技术对催化剂进行了结构表征,考察了反应条件和催化剂组成对催化活性的影响。结果表明:以甲苯为溶剂,O2为氧化剂,353K反应5h,在Mn-Al复合氧化物中,Mn2Al催化剂的苯甲醇转化率达36.6%;在Cu-Mn-Al复合氧化物催化剂中,Cu0.3Mn0.7Al2催化剂的苯甲醇转化率达40.9%。各催化剂上的苯甲醛选择性均为100%。进一步研究表明:催化剂活性与其H2还原性和O2吸附性有关,高活性的催化剂表面易于吸附和活化氧分子,生成活性氧物种,参与氧化反应。 |
英文摘要: |
A series of Mn-Al and Cu-Mn-Al composite oxides with different compositions were prepared by sol-gel method and applied in selective oxidation of benzyl alcohol to benzaldehyde. The catalysts were characterized by means of techniques such as X-ray diffraction (XRD), N2 physisorption (BET), Scanning electron microscope (SEM), Temperature-programmed reduction of hydrogen (H2-TPR), Temperature-programmed desorption of oxygen (O2-TPD), and X-ray photoelectron spectroscopy (XPS). The effect of reaction conditions and catalyst compositions on catalytic activity was investigated. It is shown that the high conversion of benzyl alcohol can be obtained under the following reaction conditions: O2 is used as oxidant, toluene as solvent, the content of benzyl alcohol 0.1ml, reaction temperature 353K, and reaction time 5h. Among Mn-Al composite oxides, the catalyst with composition of Mn2Al exhibits high catalytic activity, over which the conversion of benzyl alcohol reaches 36.6%. Of Cu-Mn-Al composite oxide catalysts, the Cu0.3Mn0.7Al2 with 40.9% conversion of benzyl alcohol is more active than others. Over all catalysts, the selectivity of benzaldehyde maintains 100%. The characterization data indicates that the catalyst with higher activity has more deficit oxygen, more facile adsorption and activation for oxygen to participate in the oxidation reaction of benzyl alcohol. |
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