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排序方式: 共有105条查询结果,搜索用时 15 毫秒
1.
Chrysostomos Wesdemiotis Aberra Fura Fred W. McLafferty 《Journal of the American Society for Mass Spectrometry》1991,2(6):459-463
Collisionally activated dissociation and neutralization-reionization experiments reveal that protonation of ethanol leads to two distinct isomers, the classical ion CH3CH2OH+2 and the proton-bound complex C2H4…H+…OH2. The neutral counterpart of the latter is unstable, whereas that of the former can be produced in a bound state if the CH3CH2OH+2 precursor ion is formed under low ion source pressure conditions and, thus, with higher internal energies. This suggests that there are substantial differences in the geometries of CH3CH2OH+2 and the hypervalent CH3CH2OH2 ·. This provides only a partial explanation for unusual isotope effects; C2H5OD2 ·, CH3CD2OD2 ·, and CD3CH2OD2 · are substantially more stable than C2D5OD2 · and C2H5OH2 ·. 相似文献
2.
Helmut Schwarz Chrysostomos Wesdemiotis Ferdinand Bohlmann 《Journal of mass spectrometry : JMS》1974,9(12):1223-1225
The electron-impact-induced elimination of piperidine from the title compound could be established by investigation of the unsymmetrically 2H-labelled compound. The mechanism of a 1,1-elimination can be excluded be unequivocally. 相似文献
3.
Major deficiencies of mass spectrometry for characterizing isomeric molecules, and of collisionally activated dissociation for characterizing isomeric ions, can be alleviated by complementary information from new techniques of neutraiization-reionization (NR) mass spectrometry. Mass data can be obtained from most fragments of the original species, irrespective of their ability to retain the charge; dissociation of fast neutrals prepared from isomeric ions can involve novel reaction pathways and can minimize competing isomerization reactions; isomeric neutrals undergoing similar dissociations can be differentiated by forming them with different internal energies; reionization of the neutral products to negative as well as positive ions can provide increased selectivity; and structural information on the resulting ions can be derived using MS/MS/MS, Dissociation by novel non-isomerization pathways can also be effected by a second addition (or subtraction) of an electron to produce an unstable ion of opposite charge. Special techniques can yield neutralized products in favorable dissociative states by collisional activation, by using neutralization targets of selected ionization energy, or through Franck-Condon factors. Optimum excitation of the neutral is important, as this should be high enough to minimize rearrangement, to maximize the differences in the dissociation pathways of isomers, and to minimize the further dissociation of the characteristic primary products of the neutral. NR experiments can, thus, also provide information on the energy surfaces for unimolecular dissociations of neutrals that are difficult to study by conventional techniques. Dissociations of the neutrals can be differentiated from those occurring after reionization by separate collisional activation of the neutrals, by changing the ionization energy of the neutralization agent, or by reionization to ions of opposite charge. 相似文献
4.
Strong ionic interactions in noncovalent complexes between poly(ethylene imine), a cationic electrolyte,and Cibacron Blue,a nucleotide mimic – implications for oligonucleotide vectors 下载免费PDF全文
Ömür Çelikbıçak Bekir Salih Chrys Wesdemiotis 《Journal of mass spectrometry : JMS》2014,49(7):597-607
Cationic polymers can bind DNA to form polyplexes, which are noncovalent complexes used for gene delivery into the targeted cells. For more insight on such biologically relevant systems, the noncovalent complexes between the cationic polymer poly(ethylene imine) (PEI) and the nucleotide mimicking dye Cibacron Blue F3G‐A (CB) were investigated using mass spectrometry methods. Two PEIs of low molecular weight were utilized (Mn ≈ 423 and 600 Da). The different types of CB anions produced by Na+/H+ exchanges on the three sulfonic acid groups of CB and their dehydrated counterparts were responsible for complex formation with PEI. The CB anions underwent noncovalent complex formation with protonated, but not with sodiated PEI. A higher proportion of cyclic oligomers were detected in PEI423 than PEI600, but both architectures formed association products with CB. Tandem mass spectrometry studies revealed a significantly stronger noncovalent interaction between PEI and dehydrated CB than between PEI and intact CB. Copyright © 2014 John Wiley & Sons, Ltd. 相似文献
5.
One‐Step Multicomponent Self‐Assembly of a First‐Generation Sierpiński Triangle: From Fractal Design to Chemical Reality 下载免费PDF全文
Rajarshi Sarkar Kai Guo Dr. Charles N. Moorefield Prof. Mary Jane Saunders Prof. Chrys Wesdemiotis Prof. George R. Newkome 《Angewandte Chemie (International ed. in English)》2014,53(45):12182-12185
A novel terpyridine‐based architecture that mimics a first‐generation Sierpiński triangle has been synthesized by multicomponent assembly and features tpy? CdII? tpy connectivity (tpy=terpyridine). The key terpyridine ligands were synthesized by the Suzuki cross‐coupling reaction. Mixing two different terpyridine‐based ligands and CdII in a precise stoichiometric ratio (1:1:3) produced the desired fractal architecture in near‐quantitative yield. Characterization was accomplished by NMR spectroscopy, mass spectrometry, and transmission electron microscopy. 相似文献
6.
7.
Mustafa Y. Sen Judit E. Puskas David E. Dabney Chrys Wesdemiotis Christelle Absalon 《Journal of polymer science. Part A, Polymer chemistry》2010,48(16):3501-3506
A new two‐step synthesis of polyisobutylene (PIB) with precisely one thymine functionality per chain (PIB‐T) is reported. The primary hydroxyl‐functionalized PIB (PIB‐OH) precursor was prepared by direct functionalization via living carbocationic polymerization of isobutylene initiated by the α‐methylstyrene epoxide/TiCl4 system. Matrix assisted laser desorption/ionization time‐of‐flight mass spectrometry (MALDI‐ToF MS) of a low molecular weight PIB‐OH precursor demonstrated the effectiveness of direct functionalization by this method. A PIB‐acrylate precursor (PIB‐Ac) was obtained from such a PIB‐OH, and the PIB‐T was subsequently prepared by Michael addition of thymine across the acrylate double bond. MALDI‐ToF MS of the products verified that all polymer chains carried precisely one thymine group. © 2010 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 48: 3501–3506, 2010 相似文献
8.
Jianglin Wu Chrys Wesdemiotis 《Journal of the American Society for Mass Spectrometry》2001,12(12):106
The Li atom adducts of formaldehyde (LiOCH2) and formaldimine (LiNHCH2) are produced in the gas phase by neutralization of the corresponding cations. Subsequent reionization, ca. 0.3 μs later, shows that the nominally hypervalent complexes LiXCH2 (X=O or NH) are stable, residing in potential energy minima. In the time span between the neutralization and reionization events, the LiXCH2 molecules dissociate partly into their constituents, Li + XCH2, the fragmentation extent of LiNHCH2 being more extensive. Ab initio calculations reveal three bound states for both Li atom complexes. Two (states A and B) resemble C-centered radicals carrying an ion pair, Li+·−X---CH2·, and can be viewed as lithiated derivatives of the hydroxymethyl (HOCH2·) or aminomethyl (H2NCH2·) radical; the third state (C) represents a conventional, electrostatically bonded Li---X=CH2 complex with an essentially intact X=C double bond and the unpaired electron located at the metal atom. States A and B are bound more strongly than state C for LiOCH2; the opposite is true for LiNHCH2, where C is the most stable arrangement and B only marginally bound. The larger degree of dissociation observed for LiNHCH2 vis à vis LiOCH2 upon neutralization–reionization points out that the experiment samples a considerable amount of state B which is barely bound for LiNHCH2. 相似文献
9.
10.
Michael J. Nold Blas A. Cerda Chrys Wesdemiotis 《Journal of the American Society for Mass Spectrometry》1999,10(1):1-8
Dissociation of the amide bonds in a protonated peptide leads to N-terminal sequence fragments with cyclic structures and
C-terminal sequence fragments with linear structures. The ionic fragments containing the N-terminus (b
n
) have been shown to be protonated oxazolones, whereas those containing the C-terminus (y
n
) are protonated linear peptides. The coproduced neutral fragments are cyclic peptides from the N-terminus and linear peptides
from the C-terminus. A likely determinant of these structural choices is the proton affinity (PA) of the described peptide
segments. This study determines the PA values of such segments (Pep), i.e., cyclic and linear dipeptides and a relevant oxazolone,
based on the dissociations of proton-bound dimers [Pep + B
i
]H+ in which B
i
is a reference base of known PA value (Cooks kinetic method). The dissociations are assessed at different internal energies
to thereby obtain both proton affinities as well as entropies of protonation. For species with comparable amino acid composition,
the proton affinity (and gas phase basicity) follows the order cyclic peptide ≪ oxazolone ≈ linear peptide. This ranking is
consistent with dissociation of the protonated peptide via interconverting proton-bound complexes involving N-terminal oxazolone
(O) or cyclopeptide (C) segments and C-terminal linear peptide segments (L), viz. O ⋯ H+ ⋯ L ⇄ C ⋯ H+ ⋯ L. N-terminal sequence ions (b
n
) are formed with oxazolone structures which can efficiently compete for the proton with the linear segments. On the other
hand, N-terminal neutral fragments detach as cyclic peptides, with H+ now being retained by the more basic linear segment from the C-terminus to yield y
n
. 相似文献