PFPC, School of Chemistry, The University of Melbourne, Melbourne, Victoria 3010, Australia.
J Am Chem Soc. 2010 Mar 31;132(12):4438-44. doi: 10.1021/ja100040p.
Monodisperse mesoporous anatase titania beads with high surface areas and tunable pore size and grain diameter have been prepared through a combined sol-gel and solvothermal process in the presence of hexadecylamine (HDA) as a structure-directing agent. The monodispersity of the resultant titania beads, along with the spherical shape, can be controlled by varying the amount of structure-directing agent involved in the sol-gel process. The diameter of the titania beads is tunable from approximately 320 to 1150 nm by altering the hydrolysis and condensation rates of the titanium alkoxide. The crystallite size, specific surface area (from 89 to 120 m(2)/g), and pore size distribution (from 14 to 23 nm) of the resultant materials can be varied through a mild solvothermal treatment in the presence of varied amounts of ammonia. On the basis of the results of small-angle XRD, high-resolution SEM/TEM, and gas sorption characterization, a mechanism for the formation of the monodisperse precursor beads has been proposed to illustrate the role of HDA in determining the morphology and monodispersity during the sol-gel synthesis. The approach presented in this study demonstrates that simultaneous control of the physical properties, including specific surface area, mesoporosity, crystallinity, morphology, and monodispersity, of the titania materials can be achieved by a facile sol-gel synthesis and solvothermal process.
已经通过在十六烷基胺(HDA)存在下的溶胶-凝胶和溶剂热过程制备了具有高表面积和可调节的孔尺寸和粒径的单分散介孔锐钛矿 TiO2 珠。通过改变溶胶-凝胶过程中涉及的结构导向剂的量,可以控制所得 TiO2 珠的单分散性和球形。通过改变钛醇盐的水解和缩合速率,TiO2 珠的直径可以从约 320nm 调节至 1150nm。通过在存在不同量的氨的温和溶剂热处理,可以改变所得材料的结晶度、比表面积(89 至 120m²/g)和孔径分布(14 至 23nm)。基于小角 XRD、高分辨率 SEM/TEM 和气体吸附特性的结果,提出了单分散性前驱体珠形成的机理,以说明 HDA 在溶胶-凝胶合成过程中对形态和单分散性的控制作用。本研究中提出的方法表明,通过简单的溶胶-凝胶合成和溶剂热过程可以同时控制 TiO2 材料的物理性质,包括比表面积、介孔性、结晶度、形态和单分散性。