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971.
Miao Zhang Yi Zuo Tonghui Li Min Liu Hong Yang Xinwen Guo 《American Institute of Chemical Engineers》2021,67(8):e17261
A thorough experimental investigation on the kinetic behavior of liquid-phase propylene epoxidation over TS-1 and tetrapropylammonium hydroxide (TPAOH) treated TS-1 catalysts was conducted in a fixed-bed reactor. The amounts of different coordinated Ti species in the catalysts were quantified by spectroscopies, and their catalytic performances of the epoxidation and alcoholysis of propylene oxide were measured by kinetic modeling. The study shows that the TPAOH treatment converted some of the tetrahedrally coordinated Ti to octahedrally coordinated Ti, and both species were active for the epoxidation and alcoholysis. The superior catalytic performance observed over the TPAOH treated TS-1 is due to two factors, the increased percentage of active sites, and reduced energy barrier for epoxidation on the octahedrally coordinated Ti. In addition, as the H2O2 conversion increases, the adsorption equilibrium constant of propylene oxide plays a more decisive role than the activation energy for the selectivity of propylene glycol monomethyl ethers. 相似文献
972.
Xiaonan Lu Joelle T. Reiser Benjamin Parruzot Lu Deng Igor M. Gussev Jörg C. Neuefeind Trent R. Graham Hongshen Liu Joseph V. Ryan Seong H. Kim Nancy Washton Maik Lang Jincheng Du John D. Vienna 《Journal of the American Ceramic Society》2021,104(1):183-207
High-alumina containing high-level waste (HLW) will be vitrified at the Waste Treatment Plant at the Hanford Site. The resulting glasses, high in alumina, will have distinct composition-structure-property (C-S-P) relationships compared to previously studied HLW glasses. These C-S-P relationships determine the processability and product durability of glasses and therefore must be understood. The main purpose of this study is to understand the detailed structural changes caused by Al:Si and (Al + Na):Si substitutions in a simplified nuclear waste model glass (ISG, international simple glass) by combining experimental structural characterizations and molecular dynamics (MD) simulations. The structures of these two series of glasses were characterized by neutron total scattering and 27Al, 23Na, 29Si, and 11B solid-state nuclear magnetic resonance (NMR) spectroscopy. Additionally, MD simulations were used to generate atomistic structural models of the borosilicate glasses and simulation results were validated by the experimental structural data. Short-range (eg, bond distance, coordination number, etc) and medium-range (eg, oxygen speciation, network connectivity, polyhedral linkages) structural features of the borosilicate glasses were systematically investigated as a function of the degree of substitution. The results show that bond distance and coordination number of the cation-oxygen pairs are relatively insensitive to Al:Si and (Al + Na):Si substitutions with the exception of the B-O pair. Additionally, the Al:Si substitution results in an increase in tri-bridging oxygen species, whereas (Al + Na):Si substitution creates nonbridging oxygen species. Charge compensator preferences were found for Si-[NBO] (Na+), [3]B-[NBO] (Na+), [4]B (mostly Ca2+), [4]Al (nearly equally split Na+ and Ca2+), and [6]Zr (mostly Ca2+). The network former-BO-network former linkages preferences were also tabulated; Si-O-Al and Al-O-Al were preferred at the expense of lower Si-O-[3]B and [3]B-O-[3]B linkages. These results provide insights on the structural origins of property changes such as glass-transition temperature caused by the substitutions, providing a basis for future improvements of theoretical and computer simulation models. 相似文献
973.
Long-term chemical durability of borosilicate glasses that makes them a widely accepted form of nuclear waste disposal is achieved through the formation of a porous aluminosilicate gel layer that provides passivity and limits the transport of water to the reaction front. Detailed understanding of the porous silicate gel layer is thus critical in elucidating the corrosion mechanism of these glasses and to design of new glass composition for waste immobilization and other applications. In this paper, we use the diffuse charge reactive potential to generate porous aluminosilicate glass structures with compositions equivalent to the gel layers formed at the glass-water interface with an aim to understand the processing condition on the microstructure and atomic structure of these systems. We demonstrate the use of the charge scaling techniques is an effective approach to generate these porous structures with controllable pore mophologies. After initial validation of the potentials and calcium aluminosilicate glass structures using neutron diffraction, we created gel structures with compositions similar to well-known model nuclear waste borosilicate glasses. The porosities and the pore size distribution bear a strong correlation to the processing temperature, as well as to the local atomic structure. Thus, by controlling the processing parameters, the generated porous structures can be customized to closely resemble gel structures due to borosilicate glass corrosion. These results provide insights of the micro- and atomic structure features of the porous aluminosilicate glasses and on the optimal procedure to generate porous structures that can be comparable to experimentally observed gel layer structures thus to elaborate on the correlations between the structure and phenomena in glass-water interactions. 相似文献
974.
Kang Du Yan-Bo Guo Fei Wang Jun Fan Xiao-Chuan Wang Wen-Zhong Lu Wen Lei 《Journal of the American Ceramic Society》2021,104(2):974-984
Ca1+2xSnSi2x+yO3+6x+2y (0.1 ≤ x ≤ 0.9; 0.1 ≤ y ≤ 0.9) microwave dielectric ceramics were prepared through traditional solid-state reaction sintered at 1450°C–1500°C for 5 hours. The Ca3SnSi2O9 second phase replaced the SnO2 second phase of the Ca1+2xSnSi2xO3+6x (x = 0, y = 0) ceramics by controlling the ratio of Ca:Sn:Si. The cracks of CaSnO3 (x = 0, y = 0) ceramic were inhibited, the microwave dielectric properties were optimized by introducing the Ca3SnSi2O9 second phase, and the CaSnO3-Ca3SnSi2O9 mixture system existed at (0.1 ≤ x ≤ 0.9, y = 0). The CaSnSiO5 phase with positive τf value was related to the Si-rich in CaSnSiyO3+2y (x = 0; 0.1 ≤ y ≤ 0.9), and the coexistence of three and four phases was obtained at CaSnSiyO3+2y (0.1 ≤ y ≤ 0.9) ceramics. The CaSnSiO5 phase appeared at CaSnSiyO3+2y (0.3 ≤ y ≤ 0.9) ceramics. The CaSnSiyO3+2y (y = 0.8) ceramic with 49.2 wt% CaSnSiO5 phase exhibited excellent microwave dielectric properties: εr = 11.06, Q × f = 57,500 GHz (at 11.5 GHz), and τf = +8.1 ppm/°C. 相似文献
975.
Hao Zhang Min Ge Huifeng Zhang Weijia Kong Shouquan Yu Weigang Zhang 《Journal of the American Ceramic Society》2021,104(4):1633-1640
In this study, continuous SiC-ZrB2 composite ceramic fibers were synthesized from a novel pre-ceramic polymer of polyzirconocenecarbosilane (PZCS) via melt spinning, electron beam cross-linking, pyrolysis, and finally sintering at 1800°C under argon. The ZrB2 particles with an average grain size of 30.7 nm were found to be uniformly dispersed in the SiC with a mean size of 59.7 nm, as calculated using the Scherrer equation. The polycrystalline fibers exhibit dense morphologies without any obvious holes or cracks. The tensile strength of the fibers was greater than 2.0 GPa, and their elastic modulus was ~380 GPa. After oxidation at 1200°C for 1 hour, the strength of the fibers did not decrease despite a small loss of elastic modulus. Compared to the advanced commercial SiC fibers of Tyranno SA, the fibers exhibited improved high-temperature creep resistance in the temperature range 1300-1500°C. 相似文献
976.
Qin Du Wenli Wang Zhiguang Wang Wei Su Zhiyuan Deng Jingen Wu Ming Ma Zhongqiang Hu Ziyao Zhou Ming Liu 《Journal of the American Ceramic Society》2021,104(2):896-902
Perovskite materials with compositions in the vicinity of the steep morphotropic phase boundary (MPB) exhibit various intriguing properties including giant piezoelectricity and large dielectric constant. Aside from composition, the phase configuration of the perovskites is also strongly related to the ambient temperature. Here, we report a giant piezoelectricity of 10 980 pm/V at 93°C in the 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 (PMN-PT) single crystals which is more than five times larger than that at room temperature. The enhanced piezoelectricity can be attributed to the instability of the thermally induced tetragonal phase which can be converted to the orthorhombic phase by the external electric field in the <011> oriented single crystal. The transverse piezoelectricity has been investigated by measuring the electric-field-dependent ferromagnetic resonance (FMR) field in the CoFeB/PMN-PT magnetoelectric (ME) heterostructures. The ME coupling coefficient has been increased from 49.3 to 476 Oe cm/kV as temperature increased from 25 to 90°C. The findings reveal that both longitudinal and transverse piezoelectricity in the PMN-PT single crystals can be greatly enhanced by proper setting of ambient temperature, indicating an effective route for the design of strain-mediated tunable devices with ultralow driving voltage. 相似文献
977.
Junpeng Xue Zhongkai Yu Hyeon Mi Noh Jung Hyun Jeong Byung Chun Choi Sung Heum Park Bo Ram Lee Peng Du Mingjun Song 《Journal of the American Ceramic Society》2021,104(10):5086-5098
Ce3+/Tb3+ co-doped NaMgBO3 phosphors were successfully synthesized by solid-state method. Under 381 nm excitation, the cyan emission owing to the 5d → 4f of Ce3+ ions and green emissions arising from the 5D4 → 7FJ (J = 6, 5, 4, and 3) transitions of Tb3+ ions were seen in all the phosphors. Through theoretical analysis, one knows that the energy transfer from Ce3+ to Tb3+ ions with high efficiency of 83.74% was contributed by dipole–dipole transition. Furthermore, the internal quantum efficiency of NaMgBO3:0.01Ce3+,0.03Tb3+ phosphor was 54.28%. Compared with that of at 303 K, the emission intensity of the developed products at 423 K still kept 73%, revealing the splendid thermal stability of the studied phosphors. Through utilizing the resultant phosphors as cyan-green components, the fabricated white-LED device exhibited an excellent correlated color temperature of 2785 K, high color-rendering index of 85.73, suitable luminance efficiency of 25.00 lm/W, and appropriate color coordinate of (0.4279, 0.3617). Aside from the superior photoluminescence, the synthesized phosphors also exhibited excellent cathode-luminescence properties which were sensitive to the current and accelerating voltage. Furthermore, the NaMgBO3:0.01Ce3+,0.03Tb3+ phosphors with multi-mode emissions were promising candidates for optical anti-counterfeiting. All the results indicated that the Ce3+/Tb3+ co-doped NaMgBO3 phosphors were potential multi-platforms toward white-LED, field emission displays, and optical anti-counterfeiting applications. 相似文献
978.
979.
Jin Xu Tingting Zang Ding Du Sandeep Kumar Moolchand Sharma Rahul Vaish 《Journal of the American Ceramic Society》2021,104(4):1661-1668
The BaTiO3 powder was prepared via a solid-state reaction route. It was studied for the degradation of bacterial cells, dye, and pharmaceuticals waste using ultrasonically driven piezocatalytic effect. The bacterial catalytic behavior of poled BaTiO3 was remarkably increased during ultrasonication (10% E coli survival in 60 minutes). The structural damages were illustrated using scanning electron micrographs of bacterial cells which demonstrated morphological manifestations under different conditions. Methylene blue (MB dye), ciprofloxacin and diclofenac were also cleaned using the piezocatalytic effect associated with the poled BaTiO3 powder. Around 92, 85, and 78% of degradations were observed within 150 minutes duration for methylene blue, ciprofloxacin, and diclofenac, respectively. 相似文献
980.
Polyhedral oligomeric silsesquioxane (POSS) as an organic–inorganic hybrid at a molecular level, has excellent mechanical properties, thermodynamic properties, dielectric properties and so on. In recent decades, POSS has been extensively used in modification of various polymers to prepare nanocomposites with enhanced comprehensive performances. Biomass materials such as chitosan, cellulose, silk protein, collagen fibers and gelatin have excellent biocompatibility and biodegradability, which have been widely used in the fields such as biomedical, innovative environmental protection and so on. However, deficiencies including insufficient mechanical properties and rapid rate of biodegradation hampered their application. This paper briefly introduced the principal methods to synthesize POSS nanoparticles, and then focused on technologies for preparing biomass-based composites utilizing diverse functional POSSs. Finally, put forward the prospects of POSS modification technology and its future application direction. This article will have a positive guiding role for the further research and development of biomass/POSS nanocomposites. 相似文献