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71.
Luis Miaja‐Avila Galen C. O'Neil Young Il Joe Kelsey M. Morgan Joseph W. Fowler William B. Doriese Brianna Ganly Deyu Lu Bruce Ravel Daniel S. Swetz Joel N. Ullom 《X射线光谱测定》2021,50(1):9-20
X‐ray emission spectroscopy (XES) of transition metal compounds is a powerful tool for investigating the spin and oxidation state of the metal centers. Valence‐to‐core (vtc) XES is of special interest, as it contains information on the ligand nature, hybridization, and protonation. To date, most vtc‐XES studies have been performed with high‐brightness sources, such as synchrotrons, due to the weak fluorescence lines from vtc transitions. Here, we present a systematic study of the vtc‐XES for different titanium compounds in a laboratory setting using an X‐ray tube source and energy dispersive microcalorimeter sensors. With a full‐width at half‐maximum energy resolution of approximately 4 eV at the Ti Kβ lines, we measure the XES features of different titanium compounds and compare our results for the vtc line shapes and energies to previously published and newly acquired synchrotron data as well as to new theoretical calculations. Finally, we report simulations of the feasibility of performing time‐resolved vtc‐XES studies with a laser‐based plasma source in a laboratory setting. Our results show that microcalorimeter sensors can already perform high‐quality measurements of vtc‐XES features in a laboratory setting under static conditions and that dynamic measurements will be possible in the future after reasonable technological developments. 相似文献
72.
Mass spectrometry (MS) based proteomics has brought a radical approach to systems biology, offering a platform to study complex biological functions. However, key proteomic technical challenges remain, mainly the inability to characterise the complete proteome of a cell due to the thousands of diverse, complex proteins expressed at an extremely wide concentration range. Currently, high throughput and efficient techniques to unambiguously identify and quantify proteins on a proteome-wide scale are in demand. Miniaturised analytical systems placed upstream of MS help us to attain these goals. One time-consuming step in traditional techniques is the in-solution digestion of proteins (4-20 h). This also has other drawbacks, including enzyme autoproteolysis, low efficiency, and manual operation. Furthermore, the identification of α-helical membrane proteins has remained a challenge due to their high hydrophobicity and lack of trypsin cleavage targets in transmembrane helices. We demonstrate a new rapidly produced glass/PDMS micro Immobilised Enzyme Reactor (μIMER) with enzymes covalently immobilised onto polyacrylic acid plasma-modified surfaces for the purpose of rapidly (as low as 30 s) generating peptides suitable for MS analysis. This μIMER also allows, for the first time, rapid digestion of insoluble proteins. Membrane protein identification through this method was achieved after just 4 min digestion time, up to 9-fold faster than either dual-stage in-solution digestion approaches or other commonly used bacterial membrane proteomic workflows. 相似文献
73.
Crystallization of a semi-crystalline polyolefin in the presence of low molecular weight modifiers was quantified by differential scanning calorimetry and optical microscopy. The polyolefin was a commercial grade of isotactic poly(1-butene) (iPB). Two modifiers were used: an oligomeric plasticizer, designated HOAO, which decreased the glass transition temperature (Tg) of the system, and an oligomeric tackifier, designated HOCP, which increased Tg. Binary iPB/modifier blends containing 10% or 20% by weight of HOAO or HOCP were examined to determine how their addition affects Tg, while ternary iPB/HOAO/HOCP blends containing 10% or 20% by weight of total modifier were examined to determine the effects of dilution by using a ratio of HOAO to HOCP that matched the Tg of iPB. The addition of modifier decreased the nucleation rate, spherulitic crystal growth rate, and final crystallinity of each blend. However, only the nucleation rate showed a dependence on the type of modifier, with nucleation retarded more by HOCP than by HOAO. A Hoffman-Weeks analysis of the melting point as a function of crystallization temperature confirmed that the driving force for nucleation was reduced, and that the effect was larger for HOCP. An Avrami analysis of the bulk crystallization kinetics was consistent with these observations, as the Avrami exponents were in the range of 3-4. 相似文献
74.
We have directly resolved shock structures in pure aluminum in the first few hundred picoseconds subsequent to a dynamic load at peak stresses up to 43 GPa and strain rates in excess of 10(10) s(-1). For strong shocks we obtain peak stresses, strain rates, and rise times. From these data, we directly validate the invariance of the dissipative action in the strong shock regime, and by comparing with data obtained at much lower strain rates show that this invariance is observed over at least 5 orders of magnitude in the strain rate. Over the same range, we similarly validate the fourth-power scaling of the strain rate with the peak stress (the Swegle-Grady relation). 相似文献
75.
76.
Márcia R. S. Silva Mary C. F. Alves S. J. G. Lima L. E. B. Soledade Elaine C. Paris E. Longo A. G. Souza Iêda M. G. Santos 《Journal of Thermal Analysis and Calorimetry》2009,97(2):559-564
Sr(Ti,Nd)O3 was synthesized in order to evaluate the influence of the amount of neodymium on the thermal and structural properties of
SrTiO3. The synthesis was carried out using the polymeric precursor method. A small mass gain was observed for the SrTiO3 and SrTi0.98Nd0.02O3 samples accompanied by an exothermic peak in the DTA curves. Other steps at higher temperatures are assigned to the combustion
of the organic material and carbonate. Elimination of defects by previous calcination of the precursors is responsible by
the short and long range ordering of the perovskite. Cubic phase was obtained for undoped and doped SrTiO3. 相似文献
77.
In an article Cheng (2009) [3] published recently in this journal, it was shown that when k≥3, the problem of deciding whether the distinguishing chromatic number of a graph is at most k is NP-hard. We consider the problem when k=2. In regards to the issue of solvability in polynomial time, we show that the problem is at least as hard as graph automorphism, but no harder than graph isomorphism. 相似文献
78.
J. P. Bocquet R. Brissot H. R. Faust M. Fowler J. Wilhelmy M. Asghar M. Djebara 《Zeitschrift für Physik A Hadrons and Nuclei》1990,335(1):41-48
The mass and nuclear charge distributions of fission fragments from229Th(nth, f) have been measured at several kinetic energies with the mass spectrometer Lohengrin (ILL-Grenoble). The average proton e-o effect, which reaches 41%, induces large oscillations in the parameters of the isotopic charge distribution. A comparison of the data from different fissile nuclei shows the importance of the last stage of the process for intrinsic excitations. 相似文献
79.
David B. Redmond Charles M. Quinn Patrick W. Fowler 《Journal of mathematical chemistry》1998,23(3-4):263-276
Some new aspects of qualitative molecular-orbital theory are developed within the context of group theory and a symmetrized
Hückel approximation. Conclusions concerning the eigenvalue sums for sets of eigenfunctions of the same symmetries, the occurrence
of repetitions of symmetry-adapted projections and the relations between eigenvalues of Γg and Γu symmetries are exemplified using the 120 cage structure of Ih point symmetry. The implications of the orbit-by-orbit approach are outlined for larger clusters.
This revised version was published online in July 2006 with corrections to the Cover Date. 相似文献
80.
Legido-Quigley C McDermott L Vilca-Melendez H Murphy GM Heaton N Lindon JC Nicholson JK Holmes E 《Electrophoresis》2011,32(15):2063-2070
Bile flow restoration is a crucial step in the recovery process post transplantation of the liver. Here, metabolic trajectories based on changes in bile secretion - a known marker of functionality - have been utilised as an approach for discovering bile fluxes during transplantation. A total of ten liver transplants were monitored and from these 68 bile samples from both donors and recipients were collected and analysed using ultra-performance LC-MS in combination with multivariate statistical analysis. Based on the principal component scores constructed from the total bile fingerprint, differentiation of the bile acid concentrations before and after transplantation was detected. A trend was also observed, by constructing metabolic trajectories, whereby the post-transplant profiles approached the position of pre-transplant profiles within 30-60?min of the restoration of bile secretion function. The ten major conjugated bile acid salts were measured and a significant increase in concentrations of taurocholic acid and taurochenodeoxycholic acid were seen after transplantation. In addition, the ratios of secondary bile acids detected in gall bladder and hepatic bile were measured before and after transplantation. This study suggests that bile acid ratios in the donor liver at the pre-transplant and post-transplant stage may be important and that profiling of secreted bile after transplantation may aid clinical assessment and progress post-transplantation. 相似文献