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41.
Peter E.R. Blanchard Brianna R. Slater Ronald G. Cavell Arthur Mar Andrew P. Grosvenor 《Solid State Sciences》2010,12(1):50-58
The electronic structures of the quaternary oxyarsenides LaMAsO (M = Fe, Co, Ni) were examined with X-ray photoelectron spectroscopy (XPS) and X-ray absorption near-edge spectroscopy (XANES). Interpretation of the metal 2p3/2 and arsenic 3d5/2 binding energies, as well as a satellite feature in the Co 2p XPS spectrum, suggests charges that are much less extreme than expected (i.e., not M2+ and As3?) because of the strong covalent character within the M–As bonds. As M is varied, the differing degrees of charge transfer from M to As atoms within these bonds are manifested by shifts in the As 3d5/2 binding energies and changes in the As K-edge intensities. This charge transfer is isolated within the [MAs] layer and does not influence the O 1s and La 3d XPS spectra. Fitting the experimental valence band spectra of these oxyarsenides LaMAsO yielded electron populations of states that support the formal charge assignment [La3+O2?][M2+As3?]. The mixed-metal series LaFe1?xM′xAsO (M′ = Co, Ni) was examined by XANES; analysis of the metal K- and L-edges, as well as of the Co 2p XPS satellite feature, revealed that no metal–metal charge transfer takes place. 相似文献
42.
For a graph G of order |V(G)| = n and a real-valued mapping
f:V(G)?\mathbbR{f:V(G)\rightarrow\mathbb{R}}, if S ì V(G){S\subset V(G)} then f(S)=?w ? S f(w){f(S)=\sum_{w\in S} f(w)} is called the weight of S under f. The closed (respectively, open) neighborhood sum of f is the maximum weight of a closed (respectively, open) neighborhood under f, that is, NS[f]=max{f(N[v])|v ? V(G)}{NS[f]={\rm max}\{f(N[v])|v \in V(G)\}} and NS(f)=max{f(N(v))|v ? V(G)}{NS(f)={\rm max}\{f(N(v))|v \in V(G)\}}. The closed (respectively, open) lower neighborhood sum of f is the minimum weight of a closed (respectively, open) neighborhood under f, that is, NS-[f]=min{f(N[v])|v ? V(G)}{NS^{-}[f]={\rm min}\{f(N[v])|v\in V(G)\}} and NS-(f)=min{f(N(v))|v ? V(G)}{NS^{-}(f)={\rm min}\{f(N(v))|v\in V(G)\}}. For
W ì \mathbbR{W\subset \mathbb{R}}, the closed and open neighborhood sum parameters are NSW[G]=min{NS[f]|f:V(G)? W{NS_W[G]={\rm min}\{NS[f]|f:V(G)\rightarrow W} is a bijection} and NSW(G)=min{NS(f)|f:V(G)? W{NS_W(G)={\rm min}\{NS(f)|f:V(G)\rightarrow W} is a bijection}. The lower neighbor sum parameters are NS-W[G]=maxNS-[f]|f:V(G)? W{NS^{-}_W[G]={\rm max}NS^{-}[f]|f:V(G)\rightarrow W} is a bijection} and NS-W(G)=maxNS-(f)|f:V(G)? W{NS^{-}_W(G)={\rm max}NS^{-}(f)|f:V(G)\rightarrow W} is a bijection}. For bijections f:V(G)? {1,2,?,n}{f:V(G)\rightarrow \{1,2,\ldots,n\}} we consider the parameters NS[G], NS(G), NS
−[G] and NS
−(G), as well as two parameters minimizing the maximum difference in neighborhood sums. 相似文献
43.
Mark P. Stockham Alice Griffiths Dr. Bo Dong Prof. Peter R. Slater 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(6):e202103442
Lithium garnets are promising solid-state electrolytes for next-generation lithium-ion batteries. These materials have high ionic conductivity, a wide electrochemical window and stability with Li metal. However, lithium garnets have a maximum limit of seven lithium atoms per formula unit (e.g., La3Zr2Li7O12), before the system transitions from a cubic to a tetragonal phase with poor ionic mobility. This arises from full occupation of the Li sites. Hence, the most conductive lithium garnets have Li between 6–6.55 Li per formula unit, which maintains the cubic symmetry and the disordered Li sub-lattice. The tetragonal phase, however, forms the highly conducting cubic phase at higher temperatures, thought to arise from increased cell volume and entropic stabilisation permitting Li disorder. However, little work has been undertaken in understanding the controlling factors of this phase transition, which could enable enhanced dopant strategies to maintain room temperature cubic garnet at higher Li contents. Here, a series of nine tetragonal garnets were synthesised and analysed by variable temperature XRD to understand the dependence of site substitution on the phase transition temperature. Interestingly the octahedral site cation radius was identified as the key parameter for the transition temperature with larger or smaller dopants altering the transition temperature noticeably. A site substitution was, however, found to make little difference irrespective of significant changes to cell volume. 相似文献
44.
MD. Daloar Hossain Le Thi Bao Tran Jong Myung Park Kwon Taek Lim 《Journal of polymer science. Part A, Polymer chemistry》2010,48(22):4958-4964
A new, efficient method for synthesizing stable nanoparticles with poly(ethylene oxide) (PEO) functionalities on the core surface, in which the micellization and crosslinking reactions occur in one pot, has been developed. First, amphiphilic PEO‐b‐PS copolymers were synthesized by reversible addition fragmentation chain transfer (RAFT) radical polymerization of styrene using (PEO)‐based trithiocarbonate as a macro‐RAFT agent. The low molecular weight PEO‐b‐PS copolymer was dissolved in isopropyl alcohol where the block copolymer self‐assembled as core‐shell micelles, and then the core‐shell interface crosslink was performed using divinylbenzene as a crosslinking agent and 2,2′‐azobisisobutyronitrile as an initiator. The design of the amphiphilic RAFT agent is critical for the successful preparation of core‐shell interface crosslinked micellar nanoparticles, because of RAFT functional groups interconnect PEO and polystyrene blocks. The PEO functionality of the nanoparticles surface was confirmed by 1H NMR and FTIR. The size and morphology of the nanoparticles was confirmed by scanning electron microscopy, transmission electron microscopy, and dynamic laser light scattering analysis. © 2010 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2010 相似文献
45.
MD. Anwarul Hasan Carlos F. Lange Malcolm L. King 《ournal of non Newtonian Fluid Mechanics》2010,165(21-22):1431-1441
The effect of viscoelastic properties and surface tension of artificial mucus simulant samples on the size distribution and volume concentration of bioaerosol droplets generated during simulated coughing was investigated through in vitro experiments. The mucus simulant samples had viscoelastic properties in a similar range as those of real human airway mucus. The mucus simulant gels were prepared by mixing various proportions of 0.5–1.7% locust bean gum solution and 0.1 M sodium tetraborate (XLB) solution. Surface tension of one set of samples was varied by adding different amounts of SDS (sodium dodecyl sulfate) surfactant while the measurement of surface tension was performed using ADSA (axisymmetric drop shape analysis) method. The viscoelastic properties of the samples were measured using a Bohlin Gemini 200 HR (Malvern, UK) nano-rheometer with peltier plate assembly. An artificial cough machine was used to simulate human cough, generating aerosol droplets in a model trachea attached to the front of the cough machine. The size distribution and volume concentration of the droplets generated through simulated cough were measured using a laser diffraction particle sizer (SprayTec, Malvern, USA). The surface tension was found to have negligible effect on the characteristic of generated droplets within the range of this investigation. The experimental results showed a decrease in particle size as the samples changed from a viscous fluid type to a viscoelastic to an elastic solid type sample. The volume concentration also changed significantly as the viscoelasticity of the samples was varied. 相似文献
46.
Frontispiece: Surface Segregated AgAu Tadpole‐Shaped Nanoparticles Synthesized Via a Single Step Combined Galvanic and Citrate Reduction Reaction 下载免费PDF全文
47.
48.
In this paper we report the successful incorporation of silicon into SrMO(3) (M = Co, Mn) leading to a structural change from a hexagonal to a cubic perovskite. For M = Co, the cubic phase was observed for low doping levels (3%), and these doped phases showed very high conductivities (up to ≈350 Scm(-1) at room temperature). However, annealing studies at intermediate temperatures (700-800 °C), indicated that the cubic phase was metastable with a gradual transformation to a hexagonal cell on annealing. Further work showed that co-doping with Fe resulted in improved stability of the cubic phase; a composition SrCo(0.85)Fe(0.1)Si(0.05)O(3-y) displayed good stability at intermediate temperatures and a high conductivity (≈150 Scm(-1) at room temperature). For M = Mn, the work showed that higher substitution levels were required to form the cubic perovskite (≈15% Si doping), although in these cases the phases were shown to be stable to annealing at intermediate temperatures. Conductivity measurements again showed an enhancement in the conductivity on Si doping, although the conductivities were lower (≈0.3-14 Scm(-1) in the range 20-800 °C) than the cobalt containing systems. The conductivities of both systems suggest potential for use as cathode materials in solid oxide fuel cells. 相似文献
49.
Daniel Hewitt Tom Pope Misbah Sarwar Alessandro Turrina Ben Slater 《Chemical science》2022,13(44):13178
The production of widely used polymers such as polyester currently relies upon the chemical separation of and transformation of xylene isomers. The least valuable but most prevalent isomer is meta-xylene which can be selectively transformed into the more useful and expensive para-xylene isomer using a zeolite catalyst but at a high energy cost. In this work, high-throughput screening of existing and hypothetical zeolite databases containing more than two million structures was performed, using a combination of classical simulation and deep neural network methods to identify promising materials for selective adsorption of meta-xylene. Novel anomaly detection techniques were applied to the heavily biased classification task of identifying structures with a selectivity greater than that of the best performing existing zeolite, ZSM-5 (MFI topology). Eight hypothetical zeolite topologies are found to be several orders of magnitude more selective towards meta-xylene than ZSM-5 which may provide an impetus for synthetic efforts to realise these promising materials. Moreover, the leading hypothetical frameworks identified from the screening procedure require a markedly lower operating temperature to achieve the diffusion seen in existing materials, suggesting significant energetic savings if the frameworks can be realised.A combination of machine learning and high throughput simulation has identified several potential zeolite structures that appear to outperform the leading commercially used material and explained the key factors for high selectivity. 相似文献
50.
Using Monte Carlo simulations, we have found that there is a surprising non-monotonic dependence of a polymer's diffusion coefficient upon the degree of disorder of the surrounding environment. Starting with a two-dimensional periodic lattice of obstacles, we randomly displace obstacles to create a quenched gel system with a tunable degree of disorder. Very small displacements increase the diffusion coefficient of polymers since they increase the width of the tube through which the polymer chains reptate. As we displace the obstacles further, however, entropic trapping is observed and the diffusion coefficient of the polymer decreases dramatically. This is a striking example of the delicate balance between entropic and frictional effects for a polymer diffusing in a dense system. 相似文献