| 梁俊杰,董俊,咸漠,赵国明.无碱条件下Au/ZnO选择性催化氧化1,3-丙二醇合成3-羟基丙酸甲酯[J].分子催化,2014,(6):524-534 |
| 无碱条件下Au/ZnO选择性催化氧化1,3-丙二醇合成3-羟基丙酸甲酯 |
| The Base-free and Selective Oxidative Transformation of 1,3-Propanediol into Methyl 3-Hydroxypropionate by Au/ZnO Catalyst |
| 投稿时间：2014-09-15 修订日期：2014-11-07 |
| DOI： |
| 中文关键词: 金 氧化锌 1,3-丙二醇 3-羟基丙酸甲酯 选择性氧化 |
| 英文关键词:Gold ZnO 1,3-propanediol Methyl 3-hydroxypropionate Selective oxidative transformation |
| 基金项目:国家杰出青年科学基金;中国科学院知识创新项目 |
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| 中文摘要: |
| 采用溶胶-沉积法合成了高选择性的Au/ZnO催化剂，用于1,3-丙二醇选择性氧化酯化为3-羟基丙酸甲酯的反应。研究了保护剂PVA用量、金溶胶合成温度、金负载量及催化剂循环利用对反应的影响，且优化了反应温度和反应压力， 并对催化剂进行了XRD和TEM表征。结果表明，PVA:Au (m/m) = 1:4、金溶胶合成温度25℃、金负载量1w%的Au/ZnO对目标反应的催化活性最好，在100℃和pO2 = 2 MPa的条件下1,3-丙二醇的转化率达82.8%，产物3-羟基丙酸甲酯的选择性达95.4%。Au纳米粒子的粒径影响 催化性能，在Au平均粒径为2.8～6.1 nm的范围内，产物选择性随Au纳米粒子的粒径的减小而增大，平均粒径在2.8～4.8 nm的范围内时，催化剂具有较好的产物选择性(大于90%)；Au/ZnO催化剂循环利用4次后催化性能(转化率和选择性)无明显下降；并推测了无碱条件下Au/ZnO选择性催化氧化1,3-丙二醇合成3-羟基丙酸甲酯的反应机制。 |
| 英文摘要: |
| ZnO-supported gold catalysts were prepared by the sol-immobilisation method and used in the reaction of selective oxidative transformation of 1,3-propanediol into methyl 3-hydroxypropionate. The amount of protective agents (PVA) and the reduction temperature as well as the Au loading were investigated. The catalysts were also continuously used by filtering and collecting the Au/ZnO from the previous reaction mixture in the recycling tests. The reaction temperature and oxygen pressure also be optimized. The samples were characterized by powder X-ray diffraction (XRD) and transmission electron microscopy (TEM). The results show that Au/ZnO prepared at PVA:Au = 1:4 (m/m), gold-sol preparation temperature 25℃ and Au loading 1w% present the best catalytic performance for the target reaction. At 100℃ and pO2 = 2 MPa, the conversion of 1,3-propanediol were 82.8% and the selectivity of methyl 3-hydroxypropionate were 95.4%. The size of Au nanoparticles on the catalyst significantly affect the catalytic performance. When the average particle size of Au nanoparticles in the range of 2.8～6.1 nm, the selectivity of product increase with the decrease of the Au particle size. The catalyst has a good product selectivity (＞90%) when the average particle size of Au nanoparticles in the range of 2.8～4.8 nm. The Au/ZnO was recycled without a decrease in the conversion and selectivity after 4 runs. The reaction mechanism also be proposed. |
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