RESUMEN
As efficient and stable nuclear waste forms, single-phase uranium (U6+)-incorporated La2Zr2O7 nanoparticles were designed and synthesized in an air atmosphere. To obtain a high U loading, divalent magnesium (Mg2+) was introduced to balance the extra charge from the substitution of tetravalent zirconium (Zr4+) by U6+ with a minimized impact to the lattice. There is a composition-driven phase transition from order pyrochlore to defect fluorite as the U concentration increases from 10 to 30 mol %, demonstrating both good solubility and stability of the La2Zr2O7 host for U and potentially for other actinides. La2(UxMgxZr1-2x)2O7 (x = 0-0.3) nanoparticles showed good dispersity and crystallinity with an average particle size of â¼48 nm. Furthermore, X-ray photoelectron spectroscopy, Raman spectroscopy, and emission spectroscopy revealed that U was stabilized in the hexavalent state in the form of a UO22+ ion. Spectroscopic methods also demonstrated that our samples caused a scintillating response with an orange emission (597 nm) by 230 nm excitation. In addition, density functional theory simulations were employed to investigate the atomic structures and electronic properties of the U-incorporated pyrochlores. The calculated bond lengths, atomic charges, and charge density confirm the existence of UO22+ ions. Supported by both experimental and computational results, a novel geometrical structure was proposed to explain the Mg2+-U6+ substitution. This work demonstrated the successful development of U-incorporated La2Zr2O7 nanoparticles and provided an efficient way to immobilize U in these ceramic waste matrixes.
RESUMEN
Single-phase nano-crystalline yttria-stabilized zirconia (YSZ) powder was prepared by co-precipitation method using zirconium oxychloride (ZrOCl2 · 8H2O) and yttrium nitrate (Y(NO3)3 · 6H2O) as raw materials and ammonium bicarbonate (NH4HCO3) and liquor ammonia (NH4OH) as the precipitators. In order to get the powder with favorable dispersibility, polyethylene glycol (PEG, HO(CH2CH2O) n H) with different molecular weights and amounts was used as a dispersant agent in the synthesis process and its effects on the YSZ powder was investigated. The scanning electron micrograph (SEM) images showed that the degree of agglomeration and the mean crystal size of YSZ powder varied with the amount and the molecular weight of PEG. The appropriate amount and molecular weight of PEG were given by comparing the dispersibility and crystal size distribution of powders. In the process, one also could find that the promotion of dispersion was insensitive to the molecular weight, and all PEG (4002000) can exert an ability to reduce the agglomeration. The proper amount of PEG400, PEG600, PEG1000, PEG2000 was 3 wt%, 3 wt%, 2 wt%, 2 wt%, respectively. The transmission electric microscope studies in conjunction with the XRD analyzes verified the low degree of agglomeration and the size of YSZ powder varied between 10~20 nm.
RESUMEN
3D printing of transparent ceramics has attracted great attention recently but faces the challenges of low transparency and low printing resolution. Herein, magnesium aluminate spinel transparent ceramics with transmittance reaching 97% of the theoretical limit are successfully fabricated using a stereolithography-based 3D printing method assisted by hot isostatic pressing and the critical factors governing the transparency are revealed. Various transparent spinel lenses and microlattices are printed at a high resolution of ≈100-200 µm. The 3D printed spinel lens demonstrates fairly good optical imaging ability, and the printed spinel diamond microlattices as a transparent photocatalyst support for TiO2 significantly enhance its photocatalytic efficiency compared with its opaque counterparts. Compared with other 3D printed transparent materials such as silica glass or organic polymers, the printed spinel ceramics have the advantages of broad optical window, high hardness, excellent high-temperature stability, and chemical resistance and therefore, have great potential to be used in various optical lenses/windows and photocatalyst supports for application in harsh environments.
RESUMEN
We investigate the ionization and displacement effects of an electron-beam (e-beam) on amorphous Gd2Zr2O7 synthesized by the co-precipitation and calcination methods. The as-received amorphous specimens were irradiated under electron beams at different energies (80 keV, 120 keV, and 2 MeV) and then characterized by X-ray diffraction and transmission electron microscopy. A metastable fluorite phase was observed in nanocrystalline Gd2Zr2O7 and is proposed to arise from the relatively lower surface and interface energy compared with the pyrochlore phase. Fast crystallization could be induced by 120 keV e-beam irradiation (beam current = 0.47 mA/cm2). The crystallization occurred on the nanoscale upon ionization irradiation at 400 °C after a dose of less than 1017 electrons/cm2. Under e-beam irradiation, the activation energy for the grain growth process was approximately 10 kJ/mol, but the activation energy was 135 kJ/mol by calcination in a furnace. The thermally activated ionization process was considered the fast crystallization mechanism.