张胜红,张杰,贾豪强,孙培永,姚志龙.介孔磷酸锡催化1,3-二羟基丙酮制备乳酸甲酯[J].分子催化,2023,37(3):241-251 |
介孔磷酸锡催化1,3-二羟基丙酮制备乳酸甲酯 |
Conversion of 1,3-Dihydroxyacetone to Methyl Lactate Catalyzed by Mesoporous Tin Phosphate |
投稿时间:2023-01-08 修订日期:2023-02-20 |
DOI:10.16084/j.issn1001-3555.2023.03.004 |
中文关键词: 乳酸甲酯 1,3-二羟基丙酮 磷酸锡 催化 构效关系 |
英文关键词:methyl lactate 1,3-dihydroxyacetone tin phosphate catalysis structure-function relationship |
基金项目:北京市教育委员会科技计划项目(KM 201910017010) |
作者 | 单位 | E-mail | 张胜红 | 北京石油化工学院 新材料与化工学院, 恩泽生物质精细化工北京市重点实验室, 北京 102617 | | 张杰 | 北京石油化工学院 新材料与化工学院, 恩泽生物质精细化工北京市重点实验室, 北京 102617 | | 贾豪强 | 北京石油化工学院 新材料与化工学院, 恩泽生物质精细化工北京市重点实验室, 北京 102617 | | 孙培永 | 北京石油化工学院 新材料与化工学院, 恩泽生物质精细化工北京市重点实验室, 北京 102617 | sunpeiyong@bipt.edu.cn | 姚志龙 | 北京石油化工学院 新材料与化工学院, 恩泽生物质精细化工北京市重点实验室, 北京 102617 | |
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中文摘要: |
以三嵌段聚合物P123为结构导向剂在水热条件下制备了介孔磷酸锡(SnPO), 采用XRD、 N2物理吸附、 TEM、 FT-IR、 Raman、 XPS和Py-IR对SnPO结构和酸性进行了表征并关联其催化1,3-二羟基丙酮(DHA)制备乳酸甲酯的性能. 结果表明: 500 ℃ 焙烧后的SnPO为层状介孔材料, 含有丰富的Lewis (L) 酸位点, 能够在温和条件下催化DHA制备乳酸甲酯. 该反应遵循平行-序列的反应路径, 需要Brønsted (B) 酸和L酸的协同参与, 且相对高的L∶B值有助于提高乳酸甲酯选择性. 此外, SnPO具有足够的结构稳定性, 有机物在其表面沉积而导致的失活可以通过500 ℃ 空气焙烧进行再生. |
英文摘要: |
Mesoporous tin phosphate (SnPO) was prepared under hydrothermal conditions in the presence of P123 triblock copolymers as structure-directing agents. The structure and physicochemical properties of SnPO were comprehensively probed by XRD, N2 physical adsorption, TEM, FT-IR, Raman, XPS and Py-IRand correlated with its performance in the catalytic conversion of 1,3-dihydroxyacetone (DHA) to methyl lactate. The results indicated that the SnPO catalysts calcined at 500 ℃ were amorphous tin phosphates with cylindrical mesopores and abundant Lewis (L) acids, contributing to efficient conversion of DHA to methyl lactate under mild reaction conditions. The overall reaction proceeds via a combination of parallel and consecutive steps, requiring the cooperation between Brønsted (B) and Lewis (L) acids and favoring methyl lactate over the SnPO catalyst with a relatively high L∶B ratio. Besides, the SnPO catalyst suffered from an incremental loss in its performance due to the increasing organic deposits on the catalyst surface, despite its stable structure in the conversion of DHA to methyl lactate. The deactivated SnPO catalyst could be roughly regenerated by calcination at 500 ℃. |
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