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61.
Kara D. Fong Helen K. Bergstrom Bryan D. McCloskey Kranthi K. Mandadapu 《American Institute of Chemical Engineers》2020,66(12):e17091
The theory of transport phenomena in multicomponent electrolyte solutions is presented here through the integration of continuum mechanics, electromagnetism, and nonequilibrium thermodynamics. The governing equations of irreversible thermodynamics, including balance laws, Maxwell's equations, internal entropy production, and linear laws relating the thermodynamic forces and fluxes, are derived. Green–Kubo relations for the transport coefficients connecting electrochemical potential gradients and diffusive fluxes are obtained in terms of the flux–flux time correlations. The relationship between the derived transport coefficients and those of the Stefan–Maxwell and infinitely dilute frameworks are presented, and the connection between the transport matrix and experimentally measurable quantities is described. To exemplify the application of the derived Green–Kubo relations in molecular simulations, the matrix of transport coefficients for lithium and chloride ions in dimethyl sulfoxide is computed using classical molecular dynamics and compared with experimental measurements. 相似文献
62.
63.
Williams CC Thang SH Hantke T Vogel U Seeberger PH Tsanaktsidis J Lepenies B 《ChemMedChem》2012,7(2):281-291
A series of well‐defined polymer–drug conjugates were prepared in order to modify the physical properties of a known cytotoxic drug, 7‐ethyl‐10‐hydroxycamptothecin (SN‐38), the active metabolite of irinotecan (CPT‐11). Reversible addition–fragmentation chain transfer (RAFT) polymerisation was used to covalently and site‐specifically append a defined N‐(2‐hydroxypropyl)methacrylamide (HPMA) polymer to SN‐38 using a graft‐from process. These poly‐HPMA–SN‐38 conjugates displayed excellent aqueous solubility and stability, whilst retaining the cytotoxic activity of the parent SN‐38. In vitro co‐culture assays containing both cancer and noncancer cell lines demonstrated the specificity of RAFT‐derived poly‐HPMA–SN‐38 conjugates for cancerous cells. The concept of post‐optimisation modification of small‐molecule drugs through a graft‐from polymer conjugation method is introduced. 相似文献
64.
Nam Binh Do Hyun Deok Jang Inki Hong Hyoung Su Han Duc Thang Le Weon Pil Tai Jae Shin Lee 《Ceramics International》2012
Effect of excess CuO additive on the sintering behavior and piezoelectric properties of Bi0.5(Na82K0.18)0.5TiO3 ceramics was investigated. The addition of small amount of excess CuO as low as 1 mol% was quite effective to lower the sintering temperature (Ts) of BNKT ceramics down to 975 °C while their piezoelectric properties were degraded by Cu doping. However, the electric field-induced strain was markedly enhanced by further addition of Nb2O5 with CuO without elevating Ts. The normalized strain Smax/Emax of 427 pm/V was obtained with a specimen sintered with 0.02 mol CuO and 0.03 mol Nb2O5 in excess. 相似文献
65.
66.
Jorge López-Cuevas Howard Jones Helen V. Atkinson 《Journal of the American Ceramic Society》2000,83(12):2913-2918
The sessile drop method has been used to determine the time dependence of the contact angle at 850°C in vacuo for Ag–28 wt% Cu, Ag–35 wt% Cu–1.5 wt% Ti, and Ag–27 wt% Cu–12 wt% In–2 wt% Ti on vitreous and devitrified fused quartz substrates. Nonwetting behavior (θ > 90°) was observed for Ag–28 wt% Cu on both substrates with no evident effect of time at temperature. The silica substrate structure, whether crystalline or amorphous, as well as its surface condition, whether smooth or rough, made no significant difference. In contrast, with Ag–35 wt% Cu–1.5 wt% Ti and Ag–27 wt% Cu–12 wt% In–2 wt% Ti the contact angle continuously decreased with time for both silica substrates, and the structure and surface condition of the substrates had a negligible effect in the case of Ag–27 wt% Cu–12 wt% In–2 wt% Ti, which produced essentially the same contact angles on both silica substrates at a given time of hold at 850°C. The contact angles produced by Ag–35 wt% Cu–1.5 wt% Ti on devitrified fused quartz were consistently higher than those produced on the vitreous substrates, with increasing holding time at 850°C. This is attributable to the presence of extensive cracks in the α-cristobalite layer at the surface of the devitrified substrates, which obstruct wetting and spreading. These results, when correlated with the wettability of preoxidized silicon carbide by the same alloys reported in previous work, could account for the adverse effect on wetting of the high-temperature silica films formed on the surface of the SiC in that work. 相似文献
67.
Shaun P. Gaus Martin P. Harmer Helen M. Chan Hugo S. Caram Nils Claussen 《Journal of the American Ceramic Society》2000,83(7):1599-1605
The general reaction behavior of the 3A process under the thermal explosion mode of synthesis has been investigated via a continuum model. The continuum model uses mass and energy balances to predict temperature difference ( T s,avg − T f ) curves, as well as profile curves of the reactant conversions and sample temperature. In particular, the effect of the dimensionless parameters associated with the rate of local heat generation (β, the thermicity factor), the activation energy (γ, the Arrhenius number), the rate of heat redistribution (α, the modified thermal diffusivity), the rate of heat transfer by convection (Bi, the Biot number or convective heat transfer parameter), and the rate of heat transfer by radiation (Ω, the radiative heat transfer parameter) were investigated. Conditions to control the reaction process, which should produce high-density final products, were determined. It was found that the overall maximum temperature may be reduced for high γ, low β, high α, and high Bi and Ω. In terms of processing conditions, this may be obtained by reducing the initial reactant concentrations, optimizing the particle size, using small sample sizes and high compaction pressure, and increasing the heat loss by using a high thermal conductivity inert gas. 相似文献
68.
Heterogeneous film‐forming latexes were prepared using two‐stage, seeded emulsion polymerization. The polymerization was performed in a calorimetric reactor with a control unit that monitored the reaction rate and controlled the charging rate of the monomers. Three types of styrene seed latexes were prepared at 70°C. The first was an unmodified polystyrene (PS) latex. The second had the molecular weight lowered by the use of carbon tetrachloride (CCl4) as a chain‐transfer agent, added at the start of the polymerization. For the third one, divinylbenzene (DVB) was used as a comonomer. DVB was added under starved conditions near the end of the polymerization to achieve crosslinked particle shells and to introduce double bonds as possible grafting sites. The second polymerization step was performed at 80°C as a batch operation in a 200‐mL calorimeter reactor. The second‐stage polymer was poly(styrene‐co‐butadiene‐co‐methacrylic acid) (S/B/MAA). A fixed S/B ratio was used together with varying small amounts of MAA. Particle morphology and particle‐size distributions were examined after the second stage using TEM after staining with osmium tetroxide. The particle morphology was found to depend on both the seed composition and the amount of MAA used in the second stage. Molecular weight and crosslinking of the DVB‐containing seed influenced the internal particle viscosity, which gave differences in the polymerization rate and the particle morphology. Crosslinking of the second‐stage polymer decreased the monomer concentration in the particles, which could be detected as a change in the slope the pressure/conversion curve. This phenomenon was used to indicate the critical conversion for crosslinking of the second‐stage polymer. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 77: 297–311, 2000 相似文献
69.
Dunmin Lin Kin Wing Kwok Helen Wong Lai-wa Chan 《Journal of the American Ceramic Society》2009,92(6):1362-1365
In this work, the double-loop-like characteristics of K0.5 Na0.5 NbO3 + x mol% K5.4 Cu1.3 Ta10 O9 ceramic and its relationships with the transition temperature, aging, and switching have been investigated. Our results reveal that the phase transition temperature is an important parameter determining the aging requirement for the ceramics to exhibit the double-loop-like characteristics. For a ceramic with a high transition temperature, e.g. the ceramic with x =0.75 (tetragonal–orthorhombic phase temperature ∼206°C), the vacancies can migrate during the crystal transformation and settle in a distribution with the same symmetry as the crystal after the transformation. As a result, defect dipoles along the polarization direction are formed and provide restoring forces to reverse the switched polarizations, and thus producing a double polarization hysteresis ( P – E ) loop. On the other hand, aging is required for a ceramic with a low transition temperature, e.g. aging at 80°C for 30 days is required for the ceramic with x =1.5 (transition temperature ∼175°C). Our results also reveal that the defect dipoles can be switched under a slow-switching electric field (<1 Hz) or at high temperatures (>100°C), thus leading to an opening of the double P – E loop. 相似文献
70.
Sergey N. Rashkeev Daniel M. Ginosar Lucia M. Petkovic Helen H. Farrell 《Catalysis Today》2009,139(4):291
Production of hydrogen by splitting of water in the thermochemical sulfur-based cycles that employs the catalytic decomposition of sulfuric acid into SO2 and O2 is of considerable interest. However, all of the known catalytic systems studied to date that consist of metal particles on oxide substrates deactivate with time on stream. To develop an understanding of the factors that are responsible for catalyst activity, we investigate the fresh activity of several platinum group metals (PGM) catalysts, including Pd, Pt, Rh, Ir, and Ru supported on titania at 850 °C and perform an extensive theoretical study (density-functional-theory-based first-principles calculations and computer simulations) of the activity of the PGM nanoparticles of different size and shape positioned on TiO2 (rutile and anatase) and Al2O3 (γ- and η-alumina) surfaces. The activity and deactivation of the catalytic systems are defined by (i) the energy barrier for the detachment of O atoms from the SOn (n = 1, 2, 3) species, and (ii) the removal rate of the products of the sulfuric acid decomposition (atomic O, S, and the SOn species) from metal nanoparticles. We show that these two nanoscale features collectively result in the observed experimental behavior. The removal rate of the reaction products is always lower than the SOn decomposition rates. The relation between these two rates explains why the “softer” PGM nanoparticles (Pd and Pt) exhibit the highest initial catalytic activity. 相似文献