| 李和健,吴藏藏,郑丽,廖卫平,徐秀峰.Cu-BTC及其衍生物在苯甲醇选择氧化反应中的催化活性[J].分子催化,2017,31(4):341-347 |
| Cu-BTC及其衍生物在苯甲醇选择氧化反应中的催化活性 |
| Selective Catalytic Oxidation of Benzyl Alcohol over Cu-BTC and Its Derivatives |
| 投稿时间：2017-06-21 修订日期：2017-07-10 |
| DOI： |
| 中文关键词: 苯甲醇选择氧化 Cu-BTC Cu-BTC衍生物 Cu@C 催化活性 |
| 英文关键词:selective catalytic oxidation of benzyl alcohol Cu-BTC Cu-BTC derivative Cu@C catalytic activity |
| 基金项目:山东省重点研发计划项目（2016GSF117003） |
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| 中文摘要: |
| 以硝酸铜和均苯三甲酸（BTC）为原料，水热合成了一种金属有机骨架化合物Cu-BTC，在水相中催化苯甲醇选择氧化反应，H2O2氧化剂，优化了Cu-BTC的晶化条件.70℃反应1 h，Cu-BTC（110C/24 h）上的苯甲醇转化率为75.4%、苯甲醛选择性83.5%，但反应后Cu-BTC骨架完全塌陷.在氮气中高温焙烧Cu-BTC，制得衍生物Cu@C，也用于催化苯甲醇氧化反应.结果表明：Cu@C催化剂重复使用5次，可维持较高的苯甲醇转化率，但苯甲醛选择性有所下降.用X射线衍射（XRD）、N2物理吸附（BET）、热分析（TG-DSC）、红外光谱（FTIR）、能量色散X射线光谱分析（EDX）等技术对催化剂进行了结构表征，发现：Cu@C在反应中生成的Cu2O促进了苯甲醛的深度氧化. |
| 英文摘要: |
| A metal organic framework compound (MOF) of Cu-BTC was hydro-thermally synthesized by using benzene tri-carboxylic acid (BTC) as organic ligand and copper nitrate as metal cation resource. Then, the oxidation of benzyl alcohol was catalyzed by Cu-BTC as-prepared under the reaction conditions:H2O2 as oxidant and water as solvent. 75.4% conversion of benzyl alcohol and 83.5% selectivity of benzaldehyde were obtained over Cu-BTC(110C/24 h) at 70℃ for 1 h. It was found that the skeleton of Cu-BTC was collapsed after reaction. Subsequently, the Cu@C was prepared by calcining Cu-BTC in nitrogen atmosphere at high temperature, and the re-usability of Cu@C catalyst in benzyl alcohol oxidation was evaluated. It was found that the conversion of benzyl alcohol could be kept at about 60%, but the selectivity of benzaldehyde decreased after five runs. In addition, Cu-BTC and Cu@C samples were characterized by XRD, BET, TG-DSC, FTIR and EDX techniques. The results show that Cu2O formed in spent Cu@C catalysts promoted the deep oxidation of benzaldehyde to benzoic acid. |
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