非晶态铁基固体碱催化剂的酯交换性能
Transesterification Performance of Amorphous Iron-Based Solid Base Catalyst
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吴辰亮 浙江工业大学绿色化学合成技术国家重点实验室培育基地, 杭州 310014  
李小青 浙江工业大学绿色化学合成技术国家重点实验室培育基地, 杭州 310014  
张荷丰 浙江工业大学绿色化学合成技术国家重点实验室培育基地, 杭州 310014  
严新焕 浙江工业大学绿色化学合成技术国家重点实验室培育基地, 杭州 310014 xhyan@zjut.edu.cn 
摘要: 通过化学还原法和共沉淀法分别制备了非晶态和晶态的FeCeOx/SiO2固体碱催化剂。与晶态的FeCeOx/SiO2相比,非晶态的FeCeOx/SiO2催化剂对梨醇酯与甲醇的酯交换活性显著提高。通过电感耦合等离子体质谱(ICP-MS)、N2吸附-脱附、透射电子显微镜(TEM)结合选区电子衍射(SAED)、X射线衍射(XRD)、X射线光电子能谱(XPS)、CO2-TPD和NH3-TPD等对催化剂进行表征。结果表明催化剂的活性与其碱性密切相关,非晶态FeCeOx/SiO2显示出相对于晶态FeCeOx/SiO2更强的碱性。使用非晶态FeCeOx/SiO2催化剂进行梨醇酯酯交换反应,在130℃下反应10 h,梨醇酯的转化率达到95%,异戊烯醇的选择性达到96%。在重复使用10次后,催化剂活性基本不变。对新鲜的和套用10次后的FeCeOx/SiO2催化剂进行X射线衍射分析,表明该催化剂在套用10次后仍未晶化,证实其具有良好的稳定性,说明该催化剂在非均相催化酯交换反应中具有应用价值。
关键词: FeCeOx/SiO2  固体碱  非晶态  酯交换
基金项目: 国家重点研发计划(No.2017YFC0210900)资助项目。
Abstract: Both amorphous and crystalline FeCeOx/SiO2 solid base catalysts were prepared by chemical reduction and co-precipitation methods, respectively. The activity of amorphous FeCeOx/SiO2 for the transesterification of prenyl acetate with methanol was remarkably enhanced compared with crystalline FeCeOx/SiO2. The catalysts were characterized by inductively coupled plasma mass spectrometry(ICP-MS), N2 adsorption-desorption, transmission electron microscopy (TEM) in combination with selected area electron diffraction (SAED), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and temperature programmed desorption (CO2-TPD and NH3-TPD). As a result, the activity of the catalysts is found to be closely related to its basicity, and the amorphous FeCeOx/SiO2 shows higher basicity. Prenyl acetate conversion of 95% and prenyl alcohol selectivity of 96% were obtained using amorphous FeCeOx/SiO2 catalyst in transesterification reaction at 130℃ for 10 h. The catalyst maintained a high level of activity after 10 cycles of testing. X-ray diffraction analyses of fresh and used FeCeOx/SiO2 catalyst demonstrated that this catalyst is exceptionally stable, which could be of value in industrial application related to heterogeneous catalytic transesterification.
Keywords: FeCeOx/SiO2  solid base  amorphous  transesterification
投稿时间:2019-07-23 修订日期:2019-12-26
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吴辰亮,李小青,张荷丰,严新焕.非晶态铁基固体碱催化剂的酯交换性能[J].无机化学学报,2020,36(4):737-746.
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