Direct synthesis of dimethyl carbonate from methanol and carbon dioxide over organotin-functionalized mesoporous benzene-silica
Direct synthesis of dimethyl carbonate from methanol and carbon dioxide over organotin-functionalized mesoporous benzene-silica
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有机锡功能化介孔苯二氧化硅上甲醇和二氧化碳直接合成碳酸二甲酯
DOI：
10.1351/pac-con-11-06-01
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发表时间：
2011-09
影响因子：
1.8
通讯作者：
Li, Ruifeng
中科院分区：
文献类型：
--
作者：
Fan, Binbin;Li, Hongyu;Fan, Weibin;Qin, Zhangfen;Li, Ruifeng
通过(MeO)2ClSi(CH2)3SnCl3、正硅酸乙酯(TEOS)和1，4-二(三乙氧基硅基)苯在Pluronic 123酸溶液中的共缩合反应合成了有机锡功能化的有序周期介孔有机硅(Ph-PMOS)。X射线衍射图和透射电子显微镜图像中观察到的(100)、(110)和(200)晶面的衍射线和平行通道表明，样品具有高度有序的六方阵列结构。在傅立叶变换红外光谱、漫反射紫外-可见光谱和核磁共振光谱中，苯基、四面体和八面体锡物种以及QN和TN物种的特征谱带的存在为苯基和(MeO)2ClSi(CH2)3SnCl3进入骨架或硅壁提供了令人信服的证据。有机锡功能化的Ph-PMOS在甲醇和二氧化碳直接合成碳酸二甲酯(DMC)方面表现出比骨架不含苯基的有机锡化介孔二氧化硅高得多的催化活性，尽管两者都具有很高的催化稳定性。这可能是由于其表面疏水性增强以及前一种样品中存在大量六配位的锡物种和微小的氧化锡簇合物所致。在所制备的有机锡功能化Ph-PMOS上得到的DMC产率随着CO2压力的增加而单调增加。该材料在重复使用时也表现出很高的催化稳定性。
Ordered periodic mesoporous benzene-silicas (Ph-PMOs) functionalized with organotin were synthesized by co-condensing (MeO)2ClSi(CH2)3SnCl3, tetraethyl orthosilicate (TEOS), and 1,4-bis(triethoxysilyl)-benzene in a Pluronic 123 acid solution. The diffraction lines for (100), (110), and (200) facets observed in their X-ray diffraction (XRD) patterns and parallel channels in their transmission electron microscopy (TEM) images show that the samples have highly ordered hexagonal array structure. The presence of bands characteristic for phenyl groups, tetrahedral and octahedral Sn species, and Qn and Tn species in their Fourier transform/infrared (FT/IR), diffuse reflectance UV–vis, and NMR spectra gives convincing evidence for the incorporation of phenyl groups and (MeO)2ClSi(CH2)3SnCl3 into the framework or silica wall. The organotin-functionalized Ph-PMOs exhibit much higher catalytic activity than organotin-functionalized mesoporous silica lacking phenyl groups in the framework, for direct synthesis of dimethyl carbonate (DMC) from methanol and CO2, although both have high catalytic stability. This may be attributed to its enhanced surface hydro-phobicity and the presence of a large number of hexa-coordinated Sn species and tiny Sn oxide clusters in the former sample. The DMC yield obtained over the prepared organotin-functionalized Ph-PMOs increases monotonically with increasing CO2 pressure. The material also exhibits high catalytic stability upon reusage.
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影响因子：
--
作者：
Rassow
通讯作者：
Rassow
影响因子：
8.6
作者：
D. Jiang;Jinsuo Gao;Qihua Yang;Jie Yang;Can Li
通讯作者：
D. Jiang;Jinsuo Gao;Qihua Yang;Jie Yang;Can Li
影响因子：
16.6
作者：
Milios, CJ;Raptopoulou, CP;Escuer, A
通讯作者：
Escuer, A
影响因子：
8.6
作者：
William J. Hunks and;G. Ozin
通讯作者：
William J. Hunks and;G. Ozin