催化作用
羟醛缩合
冷凝
化学
丙烯酸酯
有机化学
丙烯酸甲酯
羟醛反应
高分子化学
聚合物
共聚物
物理
热力学
作者
Zhe Wang,Liang Gao,Enhui Xing,Xueying Gao,Mudi Xin,Xinxin Peng,Yibin Luo,Xiaomei Shu
出处
期刊:ACS Sustainable Chemistry & Engineering
[American Chemical Society]
日期:2024-03-07
卷期号:12 (12): 4876-4886
标识
DOI:10.1021/acssuschemeng.3c07406
摘要
It is of great importance to design heterogeneous catalysts for aldol condensation of methyl acetate and formaldehyde to realize the green and sustainable production of methyl acrylate. Herein, Cs-based heterogeneous aldol condensation catalysts via incipient wetness impregnation were optimized through enhanced interaction between supports (amorphous SiO2, silicalite-1, and TS-1) and Cs sites. By various characterization techniques such as IR–OH and 133Cs magic angle spinning NMR, it was proven that Cs/TS-1 exhibited the strongest interaction between TS-1 and Cs species with the lowest preservation of −OH groups and the largest shift toward a higher field in NMR spectra after Cs modification as well as the highly dispersed Cs sites. Correspondingly, Cs/TS-1 shows the best catalytic performance in the gas aldol condensation of methyl acetate with formaldehyde. Importantly, it is effective to verify that the better catalytic performance is closely related to the Si/Ti–O–Cs active centers rather than that of Cs2O through H2O washing. The turnover number of Cs species of the Cs/TS-1 catalyst (468.9) was much higher than that of the silicon-supported Cs catalyst (Cs/S-1, 343.3; Cs/SiO2, 211.3), and the selectivity toward methyl acetate over Cs/TS-1 (81.8%) was higher than those for Cs/S-1 (73.2%) and Cs/SiO2 (75.0%).
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