Lv Hao, Xu Dongdong, Sun Lizhi, Henzie Joel, Lopes Aaron, Gu Qingyu, Yamauchi Yusuke, Liu Ben
Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, School of Chemistry and Materials Science , Nanjing Normal University , Nanjing 210023 , China.
Key Laboratory of Eco-chemical Engineering, College of Chemistry and Molecular Engineering , Qingdao University of Science and Technology , Qingdao 266042 , China.
Nano Lett. 2019 May 8;19(5):3379-3385. doi: 10.1021/acs.nanolett.9b01223. Epub 2019 Apr 16.
Mesoporous colloidal nanospheres with tailorable asymmetric nanostructures and multimetallic elemental compositions are building blocks in next-generation heterogeneous catalysts. Introducing structural asymmetry into metallic mesoporous frameworks has never been demonstrated, but it would be beneficial because the asymmetry enables the spatial control of catalytic interfaces, facilitates the electron/mass transfer and assists in the removal of poisonous intermediates. Herein, we describe a simple bottom-up strategy to generate uniform sub-100 nm multimetallic asymmetric bowl-shaped mesoporous nanospheres (BMSs). This method uses a surfactant-directed "dual"-template to control the kinetics of metal reduction on the surface of a vesicle, forming mesoporous metal islands on its surface whose spherical cone angle can be precisely controlled. The asymmetric BMS mesostructures with different spherical cone angles (structural asymmetries) and elemental compositions are demonstrated. The high surface area and asymmetric nature of the metal surfaces are shown to enhance catalytic performance in the alcohol oxidation reactions. The findings described here offer novel and interesting opportunities for rational design and synthesis of hierarchically asymmetric nanostructures with desired functions for a wide range of applications.
具有可定制不对称纳米结构和多金属元素组成的介孔胶体纳米球是下一代多相催化剂的构建单元。将结构不对称引入金属介孔框架尚未得到证实，但这将是有益的，因为不对称能够实现催化界面的空间控制，促进电子/质量传递，并有助于去除有毒中间体。在此，我们描述了一种简单的自下而上策略，以生成均匀的亚100纳米多金属不对称碗状介孔纳米球（BMS）。该方法使用表面活性剂导向的“双”模板来控制金属在囊泡表面还原的动力学，在其表面形成介孔金属岛，其球锥角可精确控制。展示了具有不同球锥角（结构不对称）和元素组成的不对称BMS介观结构。金属表面的高表面积和不对称性质在醇氧化反应中增强了催化性能。本文所述的研究结果为合理设计和合成具有所需功能的分级不对称纳米结构提供了新颖有趣的机会，可用于广泛的应用。
