A Facile Multi-interface Transformation Approach to Monodisperse Multiple-Shelled Periodic Mesoporous Organosilica Hollow Spheres
A Facile Multi-interface Transformation Approach to Monodisperse Multiple-Shelled Periodic Mesoporous Organosilica Hollow Spheres
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DOI：
10.1021/jacs.5b05369
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发表时间：
2015-06-24
影响因子：
15
通讯作者：
Lu, Guangming
中科院分区：
文献类型：
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作者：
Teng, Zhaogang;So, Xiaodan;Lu, Guangming
通过简单的方法合成定义明确且复杂的中空结构仍然是一个重大挑战。本工作通过一步水热处理连续生长的有机硅颗粒，建立了一种简便可控的多界面转化法制备单分散多壳周期性介孔有机硅（PMO）空心球。PMO多孔球具有无机-有机杂化骨架，壳层数目可控（1-4），高比表面积（类似于805 m（2）/g），可进入的有序中通道（类似于3.2 nm），大孔体积（1.0 cm（3）/g）、均匀且可调的直径（300-550 nm）、腔室尺寸（4-54 nm）和壳厚度（10-30 nm）。此外，各种有机基团（烷基，芳香族，和杂元素片段）成功地纳入多壳PMO空心球通过连续添加不同的桥接有机硅前体。值得注意的是，不同种类的有机基团在多壳PMO空心球中的分布可以精确控制，显示出巨大的应用潜力。我们认为PMO多壳中空结构的形成归因于多个高度交联的有机硅界面的形成，为PMO材料提供了一个新的和有趣的基本原理。由于其独特的结构和框架，三壳乙烷桥PMO空心球被成功地装载抗癌药物阿霉素和全氟戊烷气体，表现出良好的效果，在杀死癌细胞和超声成像。多界面转化策略有望为制备不同用途的多功能PMO提供一种简单、可控、通用、无模板的方法。
The synthesis of well-defined and complex hollow structures via a simple method is still a major challenge. In this work, a facile and controllable multi-interface transformation approach for preparation of monodisperse multi-shelled periodic mesoporous organosilica (PMO) hollow spheres has been established by a one-step hydrothermal treatment of successively grown organosilica particles. The multi-shelled PMO hollow spheres have inorganicorganic hybrid frameworks, controllable number (1-4) of shells, high surface area (similar to 805 m(2)/g), accessible ordered mesochannels (similar to 3.2 nm), large pore volume (1.0 cm(3)/g), and uniform and tunable diameter (300-550 nm), chamber size (4-54 nm), and shell thickness (10-30 nm). In addition, various organic groups (alkyl, aromatic, and heteroelement fragments) are successfully incorporated into the multi-shelled PMO hollow spheres by successively adding different bridged organosilica precursors. Notably, the distribution of different kinds of organic groups in the multi-shelled PMO hollow spheres can be precisely controlled, showing great potential for future applications. We propose that the formation of the multi-shelled PMO hollow structures is ascribed to the creation of multiple highly cross-linked organosilica interfaces, providing a new and interesting fundamental principle for PMO materials. Due to their unique structure and frameworks, triple-shelled ethane-bridged PMO hollow spheres were successfully loaded with an anti-cancer drug doxorubicin and perfluoropentane gas, which present excellent effects in the killing of cancer cells and ultrasound imaging. It is expected that the multi-interface transformation strategy provides a simple, controllable, versatile, and template-free method for preparation of various multifunctional PMOs for different applications.