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A dual-templating strategy for the scale-up synthesis of dendritic mesoporous silica nanospheres
Green Chemistry ( IF 9.8 ) Pub Date : 2017-10-30 00:00:00 , DOI: 10.1039/c7gc02139a Peng-Cheng Liu 1, 2, 3, 4, 5 , Ye-Jun Yu 1, 2, 3, 4, 5 , Bo Peng 1, 2, 3, 4, 5 , Shi-Yu Ma 1, 2, 3, 4, 5 , Tian-Yu Ning 1, 2, 3, 4, 5 , Bing-Qian Shan 1, 2, 3, 4, 5 , Tai-Qun Yang 1, 2, 3, 4, 5 , Qing-Song Xue 1, 2, 3, 4, 5 , Kun Zhang 1, 2, 3, 4, 5 , Peng Wu 1, 2, 3, 4, 5
Green Chemistry ( IF 9.8 ) Pub Date : 2017-10-30 00:00:00 , DOI: 10.1039/c7gc02139a Peng-Cheng Liu 1, 2, 3, 4, 5 , Ye-Jun Yu 1, 2, 3, 4, 5 , Bo Peng 1, 2, 3, 4, 5 , Shi-Yu Ma 1, 2, 3, 4, 5 , Tian-Yu Ning 1, 2, 3, 4, 5 , Bing-Qian Shan 1, 2, 3, 4, 5 , Tai-Qun Yang 1, 2, 3, 4, 5 , Qing-Song Xue 1, 2, 3, 4, 5 , Kun Zhang 1, 2, 3, 4, 5 , Peng Wu 1, 2, 3, 4, 5
Affiliation
We have demonstrated a facile and green way to synthesize dendritic mesoporous silica nanoparticles (DMSNs) on an ultra-large scale (kg) with cetyltrimethylammonium bromide (CTAB) and an anionic surfactant as dual templates free of organic solvents. In contrast to its co-template role in tuning the packing parameter of the surfactant molecule organization, the anionic surfactant herein acts as a more strongly competitive counterion against the adsorption of negatively charged silicate oligomers (I−) on the micelles. Based on the new understanding of the interaction between the cationic–anionic surfactant ionic pairs and the silicate oligomers, we proposed a dual template synergistically controlled micelle self-aggregated model to understand the formation mechanism of dendritic MSNs where the anionic surfactant stabilized micelles or micelle blocks are basic self-assembling building units for the formation of center-radial pore channel networks. By using one-pot in situ isomorphous substitution, the metal Ti atom can be easily incorporated into the silica frameworks of DMSNs, and the obtained Ti-DMSN catalyst shows a superior catalytic performance in the epoxidation of cyclohexene over the typical mesoporous Ti-MCM-41 silicas.
中文翻译:
树突状介孔二氧化硅纳米球放大合成的双模板策略
我们已经证明了一种简便,绿色的方法,以十六烷基三甲基溴化铵(CTAB)和阴离子表面活性剂作为不含有机溶剂的双模板,可以超大规模(kg)合成树枝状介孔二氧化硅纳米颗粒(DMSN)。与在调谐表面活性剂分子组织的堆积参数及其共同模板的作用,所述阴离子表面活性剂本文中作为防止带负电的硅酸盐低聚物的吸附更强的竞争抗衡离子(I -)上的胶束。基于对阳离子-阴离子表面活性剂离子对与硅酸盐低聚物之间相互作用的新认识,我们提出了一种双模板协同控制的胶束自聚集模型,以了解其中阴离子表面活性剂稳定胶束或胶束嵌段的树状MSN的形成机理。是用于形成中心-径向孔道网络的基本自组装建筑单元。通过一锅式原位同构取代,金属Ti原子可以轻松地掺入DMSN的二氧化硅骨架中,并且获得的Ti-DMSN催化剂在环己烯的环氧化反应中表现出比典型的中孔Ti-MCM-更好的催化性能。 41颗硅胶。
更新日期:2017-11-15
中文翻译:
树突状介孔二氧化硅纳米球放大合成的双模板策略
我们已经证明了一种简便,绿色的方法,以十六烷基三甲基溴化铵(CTAB)和阴离子表面活性剂作为不含有机溶剂的双模板,可以超大规模(kg)合成树枝状介孔二氧化硅纳米颗粒(DMSN)。与在调谐表面活性剂分子组织的堆积参数及其共同模板的作用,所述阴离子表面活性剂本文中作为防止带负电的硅酸盐低聚物的吸附更强的竞争抗衡离子(I -)上的胶束。基于对阳离子-阴离子表面活性剂离子对与硅酸盐低聚物之间相互作用的新认识,我们提出了一种双模板协同控制的胶束自聚集模型,以了解其中阴离子表面活性剂稳定胶束或胶束嵌段的树状MSN的形成机理。是用于形成中心-径向孔道网络的基本自组装建筑单元。通过一锅式原位同构取代,金属Ti原子可以轻松地掺入DMSN的二氧化硅骨架中,并且获得的Ti-DMSN催化剂在环己烯的环氧化反应中表现出比典型的中孔Ti-MCM-更好的催化性能。 41颗硅胶。