Ordered mesoporous U 3 O 8 has been synthesized by a nanocasting route using mesoporous silica (KIT-6 and SBA-15) as templates and characterized by using XRD, SEM and nitrogen adsorption/desorption techniques.Recently, there has been great interest in synthesis of various kinds of uranium based-nanomaterials, since these materials can be applied in catalysis area and may become new building blocks for the preparation of innovative nuclear fuels [1][2][3][4][5][6]. Among them, porous uranium oxides are expected to have better performance because of its large surface area and the ability to retain the fission gas into its pores as nuclear fuel [5,7,8]. U 3 O 8 , one of the most stable uranium oxides, is readily available by the calcination of many uranium oxides, oxide hydrates or uranium salts in air at 650-900 ∘ C. After the reduction of U 3 O 8 by H 2 or CO at 500-600 ∘ C, UO 2 , which is a main component of nuclear fuel, can be obtained [5].Ordered mesoporous materials have opened up many new possibilities for applications due to their controllable pore sizes, high surface areas, and various structures [9]. Synthesis of mesoporous materials has been extended from silica-based materials to non-siliceous oxide material [10,11]. Though the synthesis method on ordered mesoporous metal oxide is becoming better and perfection with stable elements, it is still a blank when dealing with pure uranium oxide materials. Herein, we report the synthesis of ordered mesoporous U 3 O 8 with different structures by a nanocasting method using two types of silica templates (KIT-6 and SBA-15). It is well-known that uranium oxide is amphoteric, so the removal of the silica template from the uranium oxide/silica composite seems to be a challenge. In the present work, we try to improve the stability of U 3 O 8 in the NaOH solution by using a pre-treatment of N 2 gas bubbling. The control of the concentration of dissolved oxygen in the alkaline solution at a very low level leads to successful removing of silica templates and finally getting the ordered mesoporous U 3 O 8 material.Ordered mesoporous silica templates (KIT-6 and SBA-15) were synthesized according to the literature [12,13]. Ordered mesoporous U 3 O 8 materials were synthesized by the nanocasting method. Briefly, molten uranyl nitrate was impregnated into the silica matrix, followed by a calcination procedure. The silica template was then removed by a N 2 -bubbled NaOH solution. Finally, the as-synthesized U 3 O 8 samples were washed by water and ethanol, and then dried at 60 ∘ C (see detailed procedures in the Supporting information). For clarification, the samples of ordered mesoporous U 3 O 8 material replicated from the KIT-6 and SBA-15 template are labelled as U 3 O 8 -KIT-6 and U 3 O 8 -SBA-15, respectively. Figure 1 shows X-ray diffraction (XRD) patterns of the ordered mesoporous silica templates (KIT-6 and SBA-15) and the replicated mesoporous uranium oxide products. As shown in Figure 1a, the KIT-6 template exhibits typical XRD peaks that are characteristic of 3-D ...