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Efficient synthesis of 3-methylindole using biomass-derived glycerol and aniline over ZnO and CeO2 modified Ag/SBA-15 catalysts
Molecular Catalysis ( IF 3.9 ) Pub Date : 2020-06-16 , DOI: 10.1016/j.mcat.2020.111038
Yi Qu , Yining Gao , Shuyi Lin , Lei Shi

An efficient mesoporous catalyst of Ag/SBA-15 modified with ZnO and CeO2 was successfully constructed with the purpose of efficiently synthesizing 3-methylindole by biomass-derived glycerol and aniline, which up to 62% yield and 75% selectivity for 3-methylindole were achieved when Ag loading was 1.00 mmol/g−1, ZnO or CeO2 content was 1.00 or 0.05 mmol/g−1, respectively. And only 3% yield decreased when the catalyst was circulated five times. The characterizations researches on N2 physical adsorption, Fourier transform infrared (FT-IR), scanning electron microscopy and energy-dispersive X-ray spectroscopy (SEM-EDX), temperature programmed reduction of hydrogen (H2-TPR), X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature programmed desorption (TPD) of NH3 and CO2, thermogravimetric and differential thermal analysis (TG-DTA) indicated that adding the promoter of ZnO to Ag/SBA-15 increased the dispersion of the silver particles significantly and controlled the aggregation of Ag nanoparticles during the reaction remarkably because doping ZnO greatly increased the polarity of the composite carrier SBA–15–ZnO and brought about the interaction between Ag and carrier enhanced. CeO2 could promote the reduction of Ag2O and suppress the formation of carbon deposition effectively. In addition, doping ZnO and CeO2 increased the number of the weak-acid centers of the SBA-15 supported Ag-based catalyst observably, thereby the catalyst of Ag/SBA-15-ZnO-–ZnO–CeO2 acquired a good selectivity. Moreover, the reaction pathway for 3-methylindole synthesis by biomass-derived glycerol and aniline was probed in depth and a reasonable route was proposed.



中文翻译:

在ZnO和CeO 2改性的Ag / SBA-15催化剂上,使用生物质衍生的甘油和苯胺高效合成3-甲基吲哚

以生物质衍生的甘油和苯胺有效合成3-甲基吲哚为目标,成功构建了一种高效的ZnO和CeO 2改性的Ag / SBA-15介孔催化剂,产率高达62%,对3-甲基吲哚的选择性为75%。当Ag的负载量为1.00 mmol / g -1时,ZnO或CeO 2的含量分别为1.00或0.05 mmol / g -1。当催化剂循环五次时,只有3%的产率下降。N 2物理吸附,傅里叶变换红外(FT-IR),扫描电子显微镜和能量色散X射线光谱(SEM-EDX),程序升温还原氢(H 2)的表征研究-TPR),X射线衍射(XRD),透射电子显微镜(TEM),NH 3和CO 2的程序升温脱附(TPD),热重和差热分析(​​TG-DTA)表明,将ZnO助催化剂加入到Ag / SBA-15显着提高了银颗粒的分散性,并在反应过程中显着控制了Ag纳米颗粒的聚集,这是因为掺杂ZnO大大增加了复合载体SBA-15-ZnO的极性,并导致了Ag与增强载体之间的相互作用。CeO 2可以促进Ag 2 O的还原并有效抑制碳沉积的形成。另外,掺杂ZnO和CeO 2明显增加了SBA-15负载的Ag基催化剂的弱酸中心数目,从而Ag / SBA-15-ZnO--ZnO-CeO 2的催化剂具有良好的选择性。此外,深入探讨了生物质衍生的甘油与苯胺合成3-甲基吲哚的反应途径,并提出了合理的途径。

更新日期:2020-06-16
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