| Zn(Al)O复合氧化物负载Au催化剂催化氧化甘油制备1,3-二羟基丙酮 |
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| 引用本文： | 柯义虎,李景云,刘春玲,董文生,刘海.Zn(Al)O复合氧化物负载Au催化剂催化氧化甘油制备1,3-二羟基丙酮[J].化工进展,2021,40(5):2581-2592. |
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| 作者姓名： | 柯义虎 李景云 刘春玲 董文生 刘海 |
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| 作者单位： | 1.北方民族大学化学与化学工程学院，化工技术基础国家民委重点实验室，宁夏 银川 750021;2.陕西师范大学化学化工学院，应用表面与胶体化学教育部重点实验室，陕西 西安 710119 |
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| 基金项目： | 国家自然科学基金(21862001);宁夏自然科学基金(2019AAC03115);宁夏低品质资源高值化利用技术研发人才小高地;北方民族大学校级重大专项(ZDZX201803) |
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| 摘 要： | 以尿素为沉淀剂，采用均匀沉积沉淀法制备了Zn(Al)O复合氧化物负载Au催化剂，并用于无碱条件下催化氧化甘油制备1,3-二羟基丙酮（DHA）反应，值得注意的是随着载体中Zn/Al摩尔比的不同，负载Au催化剂的催化活性和产物DHA的选择性呈现明显差距。结合X射线衍射（XRD）、X射线光电子能谱（XPS）、透射电镜（TEM）、CO吸附傅里叶变换红外光谱（CO吸附FTIR）等表征手段，发现载体Zn(Al)O复合氧化物中Zn/Al摩尔比会影响表面氧物种的含量并进一步会影响催化剂的催化活性和选择性。当Zn/Al摩尔比为7∶1、反应温度为80℃、氧气压力为10bar、反应2h时获得最佳的甘油转化率（58.5%）和DHA的选择性（95.3%）。同时，还考察了反应温度、反应时间、反应压力及载体的焙烧温度对催化性能的影响，并发现反应条件对催化剂的催化活性和选择性均有不同程度的影响。此外，以Au/Zn(Al)O-7∶1催化剂为基准考察了催化剂的稳定性，并通过表征手段分析了催化剂失活的主要原因。
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| 关 键 词： | 甘油 1 3-二羟基丙酮 催化 氧化 活性 选择性 催化剂载体 负载Au催化剂 |
| 收稿时间： | 2020-07-02 |
Zn(Al)O composite oxides supported Au catalysts for selective oxidation of glycerol to 1, 3-dihydroxyacetone |
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| KE Yihu,LI Jingyun,LIU Chunling,DONG Wensheng,LIU Hai.Zn(Al)O composite oxides supported Au catalysts for selective oxidation of glycerol to 1, 3-dihydroxyacetone[J].Chemical Industry and Engineering Progress,2021,40(5):2581-2592. |
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| Authors: | KE Yihu LI Jingyun LIU Chunling DONG Wensheng LIU Hai |
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| Affiliation: | 1.Key Laboratory of Chemical Engineering and Technology, State Ethnic Affairs Commission, School of Chemistry and Chemical Engineering, North Minzu University, Yinchuan 750021, Ningxia, China
2.Key Laboratory of Applied Surface and Colloid Chemistry (SNNU), MOE, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi’an 710119, Shaanxi, China |
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| Abstract: | A series of Zn(Al)O composite oxides supported Au catalysts were prepared by deposition-precipitation with urea. Interestingly, the catalysts with varied Zn/Al molar ratios showed different catalytic performance for selective catalytic oxidation of glycerol to 1,3-dihydroxyacetone (DHA) without base. The physicochemical properties of the catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), CO adsorbed Fourier transform infrared (FTIR) spectroscopy. The results showed that the molar ratio of Zn/Al in the Zn(Al)O composite metal oxide affected the content of the reactive oxygen species and in turn the catalytic activity of glycerol oxidation. When the molar ratio of Cu/Al reached 7∶1, the supported catalyst showed the best performance, i.e. the conversion of glycerol and product selectivity of DHA reached 58.5% and 95.3% respectively with the initial O2 pressure of 10bar, at 80℃ for 2h. Then, the Au/Zn(Al)O-7∶1 catalyst was used to investigate the effects of reaction temperature, reaction time, reaction pressure and calcination temperature of supports on the catalytic oxidation of glycerol and the selectivity for DHA. Additionally, we also studied the stability of the Au/Zn(Al)O-7∶1 catalyst and discussed the deactivation reasons. |
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| Keywords: | glycerol 1 3-dihydroxyacetone catalysis oxidation reactivity selectivity catalyst support supported Au catalysts |
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