Secondary Ion Mass Spectrometry of Zeolite Materials:  Observation of Abundant Aluminosilicate Oligomers Using an Ion Trap

Groenewold, Gary S.; Kessinger, G. F.; Scott, Jill R.; Gianotto, Anita K.; Appelhans, and Anthony D.; Delmore, J.E.; Avci, Recep

doi:10.1021/ac000742a

Cited by 15 publications

(9 citation statements)

References 41 publications

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“…As a result of the experimental approach, all ionized species other than those within the isolation width applied, including H 2 O and MeOH adduct ions that may be generated during the ESI process, were ejected from the ion trap and not stored for the subsequent isolation period. The gas‐phase reactions observed here are consistent with several earlier reports of hydration reactions conducted in ion trap mass spectrometers 38, 43–46. The Ag + cationized dimer species, regardless of the amino acid, were not reactive when investigated under the same experimental conditions.…”

Section: Resultssupporting

confidence: 90%

Influence of a ring substituent on the tendency to form H₂O adducts to Ag⁺ complexes with phenylalanine analogues in an ion trap mass spectrometer

et al. 2002

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In a previous report we showed that certain binary Ag(+)-amino acid complexes formed adduct ions by the attachment of a single water and methanol molecule when stored in an ion trap mass spectrometer: complexes with aliphatic amino acids and with 4-fluorophenylalanine formed the adduct ions whereas complexes with phenylalanine and tryptophan did not. In this study we compared the tendency of the Ag(+) complexes derived from phenylalanine, 4-fluorophenylalanine, 4-hydroxyphenylalanine (tyrosine), 4-bromophenylalanine, 4-nitrophenylalanine and aminocyclohexanepropionic acid to form water adducts when stored, without further activation, in the ion trap for times ranging from 1 to 500 ms. Because the donation of pi electron density to the Ag(+) ion is a likely determining factor in complex reactivity, our aim in the present study was to determine qualitatively the influence of para-position substituents on the aromatic ring on the formation of the water adducts. Our results show that the reactivity of the complexes is influenced significantly by the presence of the various substituents. Decreases in [M + Ag](+) ion abundance, and increases in adduct ion abundance, both measured as a function of storage time, follow the trend -NO(2) > -Br > -F > -OH > -H. The complex of Ag(+) with 4-nitrophenylalanine was nearly as reactive towards water as the Ag(+) complex with aminocyclohexanepropionic acid, the last being an amino acid devoid of pi character in the ring system. Collision induced dissociation of the [M + Ag](+) species derived from the amino acids produces, among other products, Ag(+) complexes with a para-substituted phenylacetaldehyde: complexes that also form adduct species when stored in the ion trap. The trends in adduct ion formation exhibited by the aldehyde-Ag(+) complex ions were similar to those observed for the precursor complexes of Ag(+) and the amino acids, confirming the influence of the ring substituent.

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Section: Resultssupporting

confidence: 90%

Influence of a ring substituent on the tendency to form H₂O adducts to Ag⁺ complexes with phenylalanine analogues in an ion trap mass spectrometer

et al. 2002

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“…These species are due to ion-molecule reactions occurring in the ion trap during isolation and are consistent with several earlier reports of hydration reactions conducted in ion trap mass spectrometers. [46][47][48][49][50][51][52] In order to determine the most probable protonation sites, the partial atomic charges for the neutral molecules, presented in Table 3, were computed using the Hamiltonean PM6 27 implemented in MOPAC2009. 28 The use of semi-empirical calculations to find the most probable protonation site has previously been reported for the particular case of flavonoids.…”

Section: Positive Ion Mode (Protonated and Sodiated Molecules)mentioning

confidence: 99%

Electrospray ionization mass spectrometric analysis of newly synthesized α,β‐unsaturated γ‐lactones fused to sugars

Madeira

Rosa

Xavier

et al. 2010

Rapid Comm Mass Spectrometry

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Knowledge of the fragmentation mechanisms of lactones and their behaviour under electrospray ionization (ESI) conditions can be extended to larger and more complex natural products that contain an alpha,beta-unsaturated gamma-lactone moiety in their structure. Moreover, little is known about the gas-phase behaviour of alpha,beta-unsaturated gamma-lactones linked or fused to sugars. Therefore, five alpha,beta-unsaturated gamma-lactones (butenolides) fused to a pyranose ring, recently synthesized compounds with potential relevance regarding their biological properties, were investigated using ESI-MS and ESI-MS/MS in both positive and negative ion modes. Their fragmentation mechanisms and product ion structures were compared. It was observed that two isomers could be unambiguously distinguished in the negative ion mode by the fragmentation pathways of their deprotonated molecules as well as in the positive ion mode by the fragmentation pathways of either the protonated or the sodiated molecule. Fragmentation mechanisms are proposed taking into account the MS/MS data and semi-empirical calculations using the PM6 Hamiltonean. The semi-empirical calculations were also very useful in determining the most probable protonation and cationization sites.

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“…Stochastic kinetic modeling was used to validate the estimated rate constants. The combined ion trap-kinetic modeling strategy has been used in the authors' laboratory for the study of the reactions of Si, Al, and Cr oxyanions with H 2 O, − H 2 S, and O 2 . , …”

Section: Introductionmentioning

confidence: 99%

Gas-Phase Hydration of U(IV), U(V), and U(VI) Dioxo Monocations

et al. 2003

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The formation of adduct ions consisting of uranium oxycations and water was studied using an ion trap-secondary ion mass spectrometer. The U(IV) and U(V) species [UO(OH)]+ and [UO2]+ were produced by bombarding the surface of UO3 using molecular primary ions, and the U(VI) species [UO2(OH)]+ was generated by O2 oxidation of [UO(OH)]+ in the gas phase. All three ions formed H2O adducts by termolecular association reactions: [UO(OH)]+ (a U(IV) species) added three water molecules, for a total of five ligands; [UO2]+ (U(V)) added three or four water molecules, for a total of five or six ligands; and [UO2(OH)]+ (U(VI)) added four water molecules for a total of six ligands. Addition of a seventh ligand was not observed in any of the systems. These analyses showed that the optimum extent of ligation increased with increasing oxidation state of the uranium metal. Hard kinetic models were fit to the time-dependent mass spectral data using adaptive simulated annealing (ASA) to estimate reaction rates and rate constants from kinetic data sets. The values determined were validated using stochastic kinetic modeling and resulted in rate data for all forward and reverse reactions for the ensemble of reactive ions present in the ion trap. A comparison of the forward rate constants of the hydration steps showed that in general, formation of the monohydrates was slow, but that hydration efficiency increased upon addition of the second H2O. Addition of the third H2O was less efficient (except in the case of [UO2]+), and addition of the fourth H2O was even more inefficient and did not occur at all in the [UO2(OH)]+ system. Reverse rate constants also decreased with increasing ligation by H2O, except in the case of [UO(OH)(H2O)4]+, which prefers to quickly revert to the trihydrate. These findings indicate that stability of the hydrate complexes [UO y H z (H2O) n ]+ increases with increasing n, until the optimum number of ligands is achieved. The results enable correlation of uranium hydration behavior with oxidation state.

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Secondary Ion Mass Spectrometry of Zeolite Materials: Observation of Abundant Aluminosilicate Oligomers Using an Ion Trap

Cited by 15 publications

References 41 publications

Influence of a ring substituent on the tendency to form H₂O adducts to Ag⁺ complexes with phenylalanine analogues in an ion trap mass spectrometer

Influence of a ring substituent on the tendency to form H₂O adducts to Ag⁺ complexes with phenylalanine analogues in an ion trap mass spectrometer

Electrospray ionization mass spectrometric analysis of newly synthesized α,β‐unsaturated γ‐lactones fused to sugars

Gas-Phase Hydration of U(IV), U(V), and U(VI) Dioxo Monocations

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Secondary Ion Mass Spectrometry of Zeolite Materials: Observation of Abundant Aluminosilicate Oligomers Using an Ion Trap

Cited by 15 publications

References 41 publications

Influence of a ring substituent on the tendency to form H2O adducts to Ag+ complexes with phenylalanine analogues in an ion trap mass spectrometer

Influence of a ring substituent on the tendency to form H2O adducts to Ag+ complexes with phenylalanine analogues in an ion trap mass spectrometer

Electrospray ionization mass spectrometric analysis of newly synthesized α,β‐unsaturated γ‐lactones fused to sugars

Gas-Phase Hydration of U(IV), U(V), and U(VI) Dioxo Monocations

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Influence of a ring substituent on the tendency to form H₂O adducts to Ag⁺ complexes with phenylalanine analogues in an ion trap mass spectrometer

Influence of a ring substituent on the tendency to form H₂O adducts to Ag⁺ complexes with phenylalanine analogues in an ion trap mass spectrometer