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171.
Niamh Holland Patrick Duggan Eleanor Owens Wayne Cummins June Frisby Helen Hughes Peter McLoughlin 《Analytical and bioanalytical chemistry》2008,391(4):1245-1253
A powerful method utilising direct probe thermal desorption GC–MS is presented for the study of molecularly imprinted polymers
(MIPs). A series of 2-aminopyridine (2-apy)-imprinted methacrylic acid–ethyleneglycol dimethacrylate (MAA–EGDMA) copolymers
were prepared under identical conditions but with varying amounts of EGDMA (crosslinking monomer). The use of appropriate
temperature programmes permitted template removal, and the subsequent assessment of polymer affinity and specificity, all
of which were found to be dependent on polymer composition and morphology. The system was sufficiently sensitive to identify
a specific response of imprinted polymers over nonimprinted counterparts. Correlations were found to exist between thermal
desorption analysis and solution phase binding, which was assessed by UV spectroscopy, where specificity was found to diminish
with decreasing EGDMA concentration. This was attributed to the increased number of free carboxyl groups in those polymers
containing a lower percentage of EGDMA. Thermal desorption profiles obtained for the analyte were found to be unaffected by
the physical and chemical properties of the solvent used for analyte reloading.
An erratum to this article can be found at 相似文献
172.
McDonough JE Mendiratta A Curley JJ Fortman GC Fantasia S Cummins CC Rybak-Akimova EV Nolan SP Hoff CD 《Inorganic chemistry》2008,47(6):2133-2141
Enthalpies of chalcogen atom transfer to Mo(N[t-Bu]Ar)3, where Ar = 3,5-C6H3Me2, and to IPr (defined as bis-(2,6-isopropylphenyl)imidazol-2-ylidene) have been measured by solution calorimetry leading to bond energy estimates (kcal/mol) for EMo(N[t-Bu]Ar)3 (E = S, 115; Se, 87; Te, 64) and EIPr (E = S, 102; Se, 77; Te, 53). The enthalpy of S-atom transfer to PMo(N[ t-Bu]Ar) 3 generating SPMo(N[t-Bu]Ar)3 has been measured, yielding a value of only 78 kcal/mol. The kinetics of combination of Mo(N[t-Bu]Ar)3 with SMo(N[t-Bu]Ar)3 yielding (mu-S)[Mo(N[t-Bu]Ar)3]2 have been studied, and yield activation parameters Delta H (double dagger) = 4.7 +/- 1 kcal/mol and Delta S (double dagger) = -33 +/- 5 eu. Equilibrium studies for the same reaction yielded thermochemical parameters Delta H degrees = -18.6 +/- 3.2 kcal/mol and Delta S degrees = -56.2 +/- 10.5 eu. The large negative entropy of formation of (mu-S)[Mo(N[t-Bu]Ar)3]2 is interpreted in terms of the crowded molecular structure of this complex as revealed by X-ray crystallography. The crystal structure of Te-atom transfer agent TePCy3 is also reported. Quantum chemical calculations were used to make bond energy predictions as well as to probe terminal chalcogen bonding in terms of an energy partitioning analysis. 相似文献
173.
174.
The 333.6-, 351.1-, and 363.8-nm lines of a cw argon ion laser are found to coincide with the BaS B1Σ+-X1Σ+ (12, 0) R(17), (6, 0) P(35), and (3, 0) R(125) transitions, respectively. Fluorescence transitions from the laser-prepared upper levels terminating in X1Σ+ V = 0–28, A1Σ+ V = 1–3, A′1Π V = 1–13, and a3Π1 V = 3–12 are assigned. These results are combined with a previous analysis of the extensively perturbed BaS A1Σ+-X1Σ+ system [R. F. Barrow, W. G. Burton, and P. A. Jones, Trans. Farad. Soc.67, 902–906 (1971)]. Every observed perturbation of the BaS A1Σ+ state is electronically and vibrationally assigned. The levels a3Π0 V = 10–13, a3Π1 V = 12–14, a3Π2 V = 15, and A′1Π V = 10–13 are sampled via their perturbations of A1Σ+ V = 0–2. Although the mutual interactions of the a3Π, A′1Π, and A1Σ+ states approach Hund's case (c) limit, a complete deperturbation is performed from a case (a) starting point. Of the five lowest energy electronic states of BaS, only b3Σ+ remains uncharacterized. Principal deperturbed molecular constants are (in cm−1, 1σ uncertainties in parentheses):
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175.
Granular flows in shear cells have been extensively studied using the Discrete Element Method (DEM) over the last two decades. These studies have typically been performed using the soft-sphere approach where deformation is assumed elastic and small relative to the characteristic grain scale. Consequently internal stresses and strains are not able to be modelled. As a first step towards addressing these limitations, we introduce a variant of DEM, the Distributed Contact DEM (DCDEM). This method models distributed normal and frictional contacts. In this initial implementation plastic deformation is not simulated and elastic deformation is simulated by permitting overlap as in traditional DEM. The method is compared against traditional DEM for a normal and oblique impact and a granular shear cell in the small deformation limit. 相似文献