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Sara Ongay Jos Hermans Andries P. Bruins Adrianus M. C. H. Nieuwendijk Hermen Overkleeft Rainer Bischoff 《Journal of the American Society for Mass Spectrometry》2013,24(1):83-91
Electron transfer dissociation (ETD) has attracted increasing interest due to its complementarity to collision-induced dissociation (CID). ETD allows the direct localization of labile post-translational modifications, which is of main interest in proteomics where differences and similarities between ETD and CID have been widely studied. However, due to the fact that ETD requires precursor ions to carry at least two charges, little is known about differences in ETD and CID of small molecules such as metabolites. In this work, ETD and CID of desmosine (DES) and isodesmosine (IDS), two isomers that due to the presence of a pyridinium group can carry two charges after protonation, are studied and compared. In addition, the influence of DES/IDS derivatization with propionic anhydride and polyethyleneglycol (PEG) reagents on ETD and CID was studied, since this is a common strategy to increase sensitivity and to facilitate the analysis by reversed-phase chromatography. Clear differences between ETD and CID of non-derivatized and derivatized-DES/IDS were observed. While CID is mainly attributable to charge-directed fragmentation, ETD is initiated by the generation of a hydrogen atom at the initial protonation site and its subsequent transfer to the pyridinium ring of DES/IDS. These differences are reflected in the generation of complex CID spectra dominated by the loss of small, noninformative molecules (NH3, CO, H2O), while ETD spectra are simpler and dominated by characteristic side-chain losses. This constitutes a potential advantage of ETD in comparison to CID when employed for the targeted analysis of DES/IDS in biological samples. Figure
A mechanistic study of electron transfer dissociation (ETD) and collision-induced dissociation (CID) of labeled and free desmosine and isodesmosine provides evidence that CID is mainly due to charge-directed fragmentation while ETD is initiated by the generation of a hydrogen atom at the initial protonation site, and its subsequent transfer to the pyridinium ring. 相似文献
34.
The non-equilibrium Richards equation is solved using a moving finite element method in this paper. The governing equation is discretized spatially with a standard finite element method, and temporally with second-order Runge–Kutta schemes. A strategy of the mesh movement is based on the work by Li et al. [R.Li, T.Tang, P.W. Zhang, A moving mesh finite element algorithm for singular problems in two and three space dimensions, Journal of Computational Physics, 177 (2002) 365–393]. A Beckett and Mackenzie type monitor function is adopted. To obtain high quality meshes around the wetting front, a smoothing method which is based on the diffusive mechanism is used. With the moving mesh technique, high mesh quality and high numerical accuracy are obtained successfully. The numerical convergence and the advantage of the algorithm are demonstrated by a series of numerical experiments. 相似文献
35.
Benisvy L Gamez P Fu WT Kooijman H Spek AL Meijerink A Reedijk J 《Dalton transactions (Cambridge, England : 2003)》2008,(24):3147-3149
The first examples of lanthanide complexes with a 2-hydroxyisophthalate ligand are reported; the blue-emitting ligand acts as a very efficient sensitizer of the Tb(III) green emissions and does so in the near-UV region. 相似文献
36.
P. Tim Prins Johanna C. van der Bok Thomas P. van Swieten Stijn O. M. Hinterding Andy J. Smith Andrei V. Petukhov Andries Meijerink Freddy T. Rabouw 《Angewandte Chemie (International ed. in English)》2023,62(28):e202305086
β-NaYF4 nanocrystals are a popular class of optical materials. They can be doped with optically active lanthanide ions and shaped into core-multi-shell geometries with controlled dopant distributions. Here, we follow the synthesis of β-NaYF4 nanocrystals from α-NaYF4 precursor particles using in situ small-angle and wide-angle X-ray scattering and ex situ electron microscopy. We observe an evolution from a unimodal particle size distribution to bimodal, and eventually back to unimodal. The final size distribution is narrower in absolute numbers than the initial distribution. These peculiar growth dynamics happen in large part before the α-to-β phase transformation. We propose that the splitting of the size distribution is caused by variations in the reactivity of α-NaYF4 precursor particles, potentially due to inter-particle differences in stoichiometry. Rate equation modeling confirms that a continuous distribution of reactivities can result in the observed particle growth dynamics. 相似文献
37.
Andries E. Brouwer Sebastian M. Cioabă Willem H. Haemers Jason R. Vermette 《Journal of Algebraic Combinatorics》2016,43(4):783-799
The simplicial rook graph \(\mathrm{SR}(m,n)\) is the graph of which the vertices are the sequences of nonnegative integers of length m summing to n, where two such sequences are adjacent when they differ in precisely two places. We show that \(\mathrm{SR}(m,n)\) has integral eigenvalues, and smallest eigenvalue \(s = \max \left( -n, -{m \atopwithdelims ()2}\right) \), and that this graph has a large part of its spectrum in common with the Johnson graph \(J(m+n-1,n)\). We determine the automorphism group and several other properties. 相似文献
38.
Asmin Andries Jef Rozenski Pieter Vermeersch Djalila Mekahli Ann Van Schepdael 《Electrophoresis》2021,42(4):402-428
The presence of a dynamic and balanced equilibrium between the production of reactive oxygen (ROS) and nitrogen (RNS) species and the in-house antioxidant defense mechanisms is characteristic for a healthy body. During oxidative stress (OS), this balance is switched to increased production of ROS and RNS, exceeding the capacity of physiological antioxidant systems. This can cause damage to biological molecules, leading to loss of function and even cell death. Nowadays, there is increasing scientific and clinical interest in OS and the associated parameters to measure the degree of OS in biofluids. An increasing number of reports using LC–MS/MS methods for the analysis of OS biomarkers can be found. Since bioanalysis is usually complicated by matrix effects, various types of cleanup procedures are used to effectively separate the biomarkers from the matrix. This is an essential part of the analysis to prepare a reproducible and homogenous solution suitable for injection onto the column. The present review gives a summary of the chromatographic methods used for the determination of OS biomarkers in both urine and plasma, serum, and whole blood samples. The first part mainly describes the biological background of the different OS biomarkers, while the second part reports examples of chromatographic methods for the analysis of different metabolites connected with OS in biofluids, covering a period from 2015 till early 2020. The selected examples mainly include LC–MS/MS methods for isoprostanes, oxidized proteins, oxidized lipoproteins, and DNA/RNA biomarkers. The last part explains the clinical relevance of this review. 相似文献
39.
Nathalie Kunkel Daniel Rudolph Andries Meijerink Stefan Rommel Richard Weihrich Holger Kohlmann Thomas Schleid 《无机化学与普通化学杂志》2015,641(7):1220-1224
Luminescence properties of divalent europium in the mixed‐anion hydride chloride EuHCl were studied for the first time. Olive‐green single crystals of EuHCl (PbFCl‐type structure: tetragonal, P4/nmm, a = 406.58(3) pm, c = 693.12(5) pm, c/a = 1.705, Z = 2) resulted from the reaction of elemental europium (Eu), sodium hydride (NaH) and sodium chloride (NaCl), while powder samples were prepared from the binary components europium dihydride (EuH2) and dichloride (EuCl2). Low temperature X‐ray powder diffraction proved the absence of phase transitions for 12(2) K ≤ T ≤ 295(2) K. Bright green emission was observed under UV‐excitation and assigned to the 4f65d1–4f7 transition of divalent europium. Temperature‐dependent luminescence absorption and emission, as well as lifetime measurements were carried out on single crystal and powder samples. Surprisingly, only limited concentration quenching was found. Additionally, two emission bands (485 and 510 nm) are observed, whose intensity ratio depends strongly on temperature. In order to explain this behavior for a single Eu2+ site, we suggest either a dynamical Jahn–Teller effect in the excited 5d1 state or emission from both a 4f65d1 state and a trapped exciton state. 相似文献
40.
van Rijssel J Erné BH Meeldijk JD Casavola M Vanmaekelbergh D Meijerink A Philipse AP 《Physical chemistry chemical physics : PCCP》2011,13(28):12770-12774
Quantum dots form equilibrium structures in liquid dispersions, due to thermodynamic forces that are often hard to quantify. Analysis of these structures, visualized using cryogenic electron microscopy, yields their formation free energy. Here we show that the nanoparticle interaction free energy can be further separated into the enthalpic and entropic contributions, using the temperature dependence of the assembled structures. Monodisperse oleic acid-capped PbSe nanoparticles dispersed in decalin were used as a model system, and the temperature-dependent equilibrium structures were imaged by cryo-TEM, after quenching from different initial temperatures. The interaction enthalpy and entropy follow from van 't Hoff's exact equation for the temperature dependence of thermodynamic equilibria, now applied to associating nanoparticles. The enthalpic component gives the magnitude of the contact interaction, which is crucial information in understanding the energetics of the self-assembly of nanoparticles into ordered structures. 相似文献