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1.
《Ceramics International》2022,48(10):14349-14359
The influence of heat-treatment temperatures (700 °C, 900°C, 1200 °C) on the phase, physical properties, crystallization rate, and in vitro properties of the solution combustion synthesized silicon-doped calcium phosphates (CaPs) were investigated. The thermodynamic aspects (enthalpy, entropy, and free energy) of the synthesis process and the crystallographic properties of the final samples were first predicted and then confirmed using density functional theory (DFT). Results demonstrated that the crystallization rate was controlled by the fuel(s) type (glycine, citric acid, and urea) and the amounts of Si4+ ions (0, 0.1, 0.4 mol). The highest calculated crystallization rate values of the un-doped, 0.1, and 0.4 mol Si-doped samples were 64%, 22%, 38%, respectively. The obtained results from the DFT simulation revealed that crystal growth in the direction of c-axis of hydroxyapatite (HAp) structure could change the stability of (001) surface of (HAp). Also, the computational data confirmed the adsorption of Si–OH groups on the (001) surface of HAp during the SCS process with an adsorption energy of 1.53 eV. AFM results in line with DFT simulation showed that the observed change in the surface roughness of Si-doped CaPs from 2 to 8 nm could be related to the doping of Si4+ ions onto the surface of CaPs. Besides, the theoretical and experimental investigation showed that crystal growth and doping of Si4+ ions could decrease the activation energy of oxygen reduction reaction (ORR). Furthermore, the results showed that the crystallized HAp structure could have great potential to efficiently reduce oxidative stress in human body. 相似文献
2.
《International Journal of Hydrogen Energy》2022,47(32):14580-14588
Recovery of hydrogen (H2) from H2-containing gas mixtures has great significance for energy conservation, cost reduction and benefit increase. However, the common separation methods have the ubiquitous problem due to phase equilibrium principle and results in the conflict between H2 concentration and H2 recovery rate in the product gas. Consequently, an innovative conception of hydrate-membrane coupling approach is proposed in this work. In the separation process, hydration and membrane permeation two separation driving forces coexist to achieve the aim of strengthening mass transfer kinetics. H2 and non-H2 components (hydrocarbons) are synchronously and directionally selected by membrane and hydrate to improve different phase compositions. Therefore, the gas in feed side could keep relatively high two separation driving forces (H2 fugacity and hydrocarbons fugacity). The results show that the coupling method could synchronously increase both the concentration and the recovery rate of H2 in the product gas. At the same time, the volume and concentration of the hydrocarbons in hydrate both increases effectively. It indicates that hydrate and membrane separation methods support each other in the separation process. The hydrate-membrane coupling method fundamentally solves the issue of the decreasing driving force resulting from single separation method and phase equilibrium relationship. 相似文献
3.
《中国稀土学报(英文版)》2022,40(7):1134-1147
In this study, the Bayan Obo rare earth concentrates mixed with Na2CO3 were used for roasting research. The phase change process of each firing stage was analyzed. The kinetic mechanism model of the continuous heating process was calculated. This study aims to recover valuable elements and optimize the production process to provide a certain theoretical basis. Using X-ray diffraction (XRD), Fourier infrared spectroscopy, scanning electron microscopy with energy dispersive spectrometry, the reaction process and the existence of mineral phases were analyzed. The variable temperature XRD and thermogravimetric method were used to calculate the roasting kinetics. The phase transition results show that carbonate-like substances first decompose into fine mineral particles, and CaO, MgO, and SiO2 react to form silicates, causing hardening. Further, REPO4 and NaF can directly generate CeF3 and CeF4 at high temperatures, and a part of CeF4 and NaF forms a solid solution substance Na3CeF7. Rare earth oxides calcined at a high temperature of 750 °C were separated to produce Ce0.6Nd0.4O1.8, Ce4O7, and LaPrO3+x. Then, BaSO4, Na2CO3, and Fe2O3 react to form barium ferrite BaFe12O19; the kinetic calculation results show that during the continuous heating process, the apparent activation energy E reaches the minimum in the entire reaction stage in the temperature range of 440–524 °C, and the reaction order n reaches the maximum, which indicates that the decomposition product REFO significantly impacts the reaction system and reduces the activation energy. The mechanism function is F(α) = [?ln (1?α)]1/3. The reaction order n reaches the minimum in the temperature range of 680–757 °C, and the apparent activation energy E is large. The difficulty of the reaction increases during the final stage. The reaction mechanism function is F(α) = [1?(1?α)1/3]2. Observing the entire reaction stage, the step of controlling the reaction rate changes from random nucleation to three-dimensional diffusion (spherical symmetry). 相似文献
4.
《Ceramics International》2022,48(9):11988-11997
We have studied peculiarities in the formation of single-crystalline barium titanate (BaTiO3) nanorods from a glycolate-mediated complex via a single-step hydrothermal process under different supersaturation (SR) conditions. X-ray diffraction (XRD) showed the formation of pure BaTiO3 with an SR of above 19. The tetragonality for the BaTiO3 (c/a) reached 1.013 at SR = 19–29 and dropped to 1.010 for SR = 39. According to the transmission electron microscopy (TEM) and XRD analyses, the rod-shaped particles exhibited single crystallinity and crystal growth along the [001] plane. With scanning electron microscopy (SEM), the morphological evolution from a plate-shaped intermediate precursor (SR = 6–9) to a rod-shaped product with an aspect ratio of 6–9 (SR = 19–29), and to non-polar material with an irregular structure (SR = 39), was observed. The negative slope, linear dependence of the particles’ width and length on the supersaturation level in the range SR = 19–39 was established for the first time. The replacement of the prevailing crystallization mechanism from in-situ topotactic transformation into dissolution-precipitation above SR = 19 was observed. It was shown that with a simple regulation of the SR, the structural and morphological characteristics of the obtained BaTiO3 nanoparticle can be effectively tuned. 相似文献
5.
Joseph Turnbull Ryan Szukalo Dmitrij Zagidulin Mark Biesinger David Shoesmith 《工业材料与腐蚀》2021,72(1-2):348-360
The strategy for the permanent disposal of high-level nuclear waste in Canada involves sealing it in a copper-coated steel container and burying it in a deep geologic repository. During the early emplacement period, the container could be exposed to warm humid air, which could result in the condensation of nitric acid, produced by the radiolysis of the humid air, on the copper surface. Previous studies have suggested that both nitrate and oxygen reduction will drive copper corrosion, with the nitrate reduction kinetics being dependent on the concentration of soluble copper(I) produced by the anodic dissolution of copper in the reaction with oxygen. This study focused on determining the kinetics of nitrate and oxygen reduction and elucidating the synergistic relationship between the two processes. This was investigated using corrosion potential and polarization measurements in conjunction with scanning electron microscopy and X-ray photoelectron spectroscopy. Oxygen reduction was shown to be the dominant cathodic reaction with the oxidation of copper(I) to copper(II) by nitrate, promoting the catalytic cycle involving the reaction of copper(II) with copper to reproduce copper(I). 相似文献
6.
Angel L. Ortiz Camila S. Rodrigues Fernando Guiberteau Yu Zhang 《Journal of the European Ceramic Society》2021,41(11):5728-5739
The microstructural development during crystallization firing of a commercially-available dental-grade nanostructured lithia-zirconia glass-ceramic (Vita Suprinity® PC) was unraveled using a wide battery of ex-situ and in-situ characterization techniques. It was found that the milling blocks are slightly crystallized glass-ceramics, with a complex chemical composition and consisting of partially de-polymerized glass plus lithium silicate (Li2SiO3) nanocrystals. It was also found that during crystallization firing the glassy matrix first reacts with part of the Li2SiO3 to form lithium disilicate (Li2Si2O5) at ~810?820 °C, and then lithium orthophosphate (Li3PO4) precipitates from the glass. This results in glass-ceramics with abundant nanocrystals embedded in a sparse zirconosilicate glass matrix (containing many other cations subsumed) that, due to its high viscosity, inhibited crystal growth. Therefore, these dental glass-ceramics are not reinforced with zirconia (ZrO2) crystals unless over-fired above ~890 °C and at the expense of its singular nanostructure. Finally, this study opens doors for optimizing the clinical performance of these dental glass-ceramics via microstructural tailoring. 相似文献
7.
Power conversion efficiency (PCE) and stability are two important properties of perovskite solar cells (PSCs). Particularly, defects in the perovskite films could cause the generation of trap states, thereby increasing the nonradiative recombination. To address this issue, suitable dopants can be incorporated to react with non-bonded atoms or surface dangling bonds to passivate the defects. Herein, we introduced TiI4 into CH3NH3PbI3 (MAPbI3) film and obtained a dense and uniform morphology with large crystal grains and low defect density. The champion cell based on 0.5% TiI4-doped MAPbI3 achieved a PCE as high as 20.55%, which is superior to those based on pristine MAPbI3 (17.64%). Moreover, the optimal solar cell showed remarkable stability without encapsulation. It retained 88.03% of its initial PCE after 300 h of storage in ambient. This work demonstrates TiI4 as a new and effective passivator for MAPbI3 film. 相似文献
8.
Sawao Honda Kento Nakashima Taketo Yoshida Yusuke Daiko Shinobu Hashimoto Yuji Iwamoto 《Journal of the American Ceramic Society》2021,104(2):1178-1187
To quantitatively investigate the initial crystallization of zeolite beta synthesized by direct heating, the extent of the reaction was precisely evaluated by X-ray diffraction measurements and Rietveld structural refinement, and a kinetic analysis of crystallization was performed using the Avrami-Erofe'ev equation. The activation energy for crystallization was lower than that for hydrothermal synthesis. Reaction and synthesis time curves revealed that the initial zeolite beta crystallization consisted of three stages. The first was an induction period with nucleation by the generation of building units and the formation of an initial coordinated structure. The second stage was crystal growth by a diffusion-controlled reaction, and the third stage involved slowing down of crystallization by the limitation of dehydrocondensation. These stages could be analyzed by calculation of the rate constant and Avrami exponent for each stage. 相似文献
9.
Dr. Santosh Shivakumaraswamy Nivedita Pandey Dr. Lionel Ballut Dr. Sébastien Violot Prof. Dr. Nushin Aghajari Prof. Dr. Hemalatha Balaram 《Chembiochem : a European journal of chemical biology》2020,21(19):2805-2817
GMP synthetase catalyses the conversion of XMP to GMP through a series of reactions that include hydrolysis of Gln to generate ammonia in the glutamine amidotransferase (GATase) domain, activation of XMP to adenyl-XMP intermediate in the ATP pyrophosphatase (ATPPase) domain and reaction of ammonia with the intermediate to generate GMP. The functioning of GMP synthetases entails bidirectional domain crosstalk, which leads to allosteric activation of the GATase domain, synchronization of catalytic events and tunnelling of ammonia. Herein, we have taken recourse to the analysis of structures of GMP synthetases, site-directed mutagenesis and steady-state and transient kinetics on the Plasmodium falciparum enzyme to decipher the molecular basis of catalysis in the ATPPase domain and domain crosstalk. Our results suggest an arrangement at the interdomain interface, of helices with residues that play roles in ATPPase catalysis as well as domain crosstalk enabling the coupling of ATPPase catalysis with GATase activation. Overall, the study enhances our understanding of GMP synthetases, which are drug targets in many infectious pathogens. 相似文献
10.
Our objective was to model the effect of mean particle size (mPS) on in vitro rumen starch degradation (IVSD) and the kinetics of gas production for different starch-based feeds. For each feed, 2 batches of the same grains were separately processed through 2 different mills (cutter or rotor speed mills), with or without different screens to achieve a wide range of mPS (0.32 to 3.31 mm for corn meals; 0.19 to 2.81 mm for barley meals; 0.16 to 2.13 mm for wheat meals; 0.28 to 2.32 mm for oat meals; 0.21 to 2.36 mm for rye meals; 0.40 to 1.79 for sorghum meals; 0.26 to 4.71 mm for pea meals; and 0.25 to 4.53 mm for faba meals). The IVSD data and gas production kinetics, obtained by fitting to a single-pool exponential model, were analyzed using a completely randomized design, in which the main tested effect was mPS (n = 6 for all tested meals, except n = 7 for corn meals and n = 5 for sorghum meals). Rumen inocula were collected from 2 fistulated Holstein dairy cows that were fed a total mixed ration consisting of 16.2% crude protein, 28.5% starch, and 35.0% neutral detergent fiber on a dry matter basis. The IVSD, evaluated after 7 h of rumen incubation, decreased linearly with increasing mPS for corn, barley, wheat, rye, pea, and faba meals, and decreased quadratically with increasing mPS for the other meals. The y-axis intercept for 7-h IVSD was below 90% starch for corn, barley, and rye feeds and greater than 90% for the other tested feeds. The mPS adjustment factors for the rate of rumen starch degradation varied widely among the different tested feeds. We found a linear decrease in starch degradation with increasing mPS for barley, wheat, rye, and pea meals, whereas we noted a quadratic decrease in starch degradation for the other tested meals. Further, we observed a linear decrease in the rate of gas production with increasing mPS in each tested feed, except for pea meal, which had a quadratic relationship. For each 1 mm increase in mPS, the gas production was adjusted by ?0.009 h?1 for corn, ?0.011 h?1 for barley, ?0.008 h?1 for wheat, and ?0.006 h?1 for faba, whereas numerically greater adjustments were needed for oat (?0.022 h?1), rye (?0.017 h?1), and sorghum (?0.014 h?1). These mPS adjustment factors could be used to modify the starch-based feed energy values as a function of mean particle size, although in vivo validation is required. 相似文献