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Tungstate ion (WO42-) confined in hydrophilic/hydrophobic nanomaterials functionalized brönsted acidic ionic liquid as highly active catalyst in the selective aerobic oxidation of alcohols in water
Molecular Catalysis ( IF 3.9 ) Pub Date : 2020-10-14 , DOI: 10.1016/j.mcat.2020.111202
Fatemeh Rajabi , Mostafa Nafe , Ghasem Rezanejad Bardajee , Rafael Luque

A Brönsted acidic Ionic Liquid containing tungstate anion functionalized polysiloxane network (PMO-IL-WO42-) was synthesized by simple self-condensation of tungstic acid and zwitterionic organosilane precursor possessing both imidazolium and sulfonate groups. Characterization by scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FT-IR), X-ray powder diffraction (XRD), thermal gravimetric analysis TGA, nitrogen porosimetry, solid-state NMR spectroscopy and elemental analysis confirmed that both imidazolium cation and tungstate anion of zwitterion are successfully incorporated inside the organosilica framework. The catalytic activity of resulting hybrid PMO-IL- WO42- material was studied in the selective aerobic oxidation of primary and secondary alcohols using an atmospheric pressure of air in pure water. Due to the ionic liquid-based charged surface containing hydrophilic sulfonic acid and tungstate group, the synergistic hydrophilic/hydrophobic and redox effect of PMO-IL-WO42- as water-friendly catalyst facilitates and enhances the activity and selectivity toward the target oxidative products in water and proved to have a particularly broad substrate scope for reliable aerobic oxidation reaction. Furthermore, the catalyst showed outstanding stability and could be easily separated and reused at least ten reactions run under the same conditions as fresh catalyst without any loss of catalytic activity and product selectivity.



中文翻译:

钨酸离子(WO 4 2-)被限制在亲水/疏水纳米材料中的功能化布朗斯台德酸性离子液体中,作为高活性催化剂,可选择性地氧化水中的酒精

含钨阴离子布朗斯台德酸性离子液体官能化聚硅氧烷网络(PMO-IL-WO 4 2 - )由钨酸和两性离子有机硅烷前体同时具有咪唑鎓和磺酸盐基团的简单的自缩合来合成。通过扫描电子显微镜(SEM),傅立叶变换红外光谱(FT-IR),X射线粉末衍射(XRD),热重分析TGA,氮气孔隙率法,固态NMR光谱和元素分析进行​​表征,证实咪唑鎓阳离子和两性离子的钨酸盐阴离子成功地掺入有机硅骨架内部。所得杂化PMO-IL-WO 4 2-的催化活性在纯水中的大气压下,对伯醇和仲醇的选择性好氧氧化进行了研究。由于含亲水性磺酸和钨酸盐基团,的协同亲水/疏水和氧化还原作用PMO-IL-WO的离子液体的基于电荷的表面4 2 -水型催化剂促进并增强朝向目标氧化活性和选择性产品被证明具有可靠的好氧氧化反应的特别广泛的底物范围。此外,该催化剂表现出优异的稳定性,并且可以容易地分离和重复使用至少十个与新鲜催化剂相同的条件下进行的反应,而不会损失任何催化活性和产物选择性。

更新日期:2020-10-15
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