Electrospray mass spectrometry applied to inorganic and organometallic chemistry

Colton, R.; D’Agostino, Antonella; Traeger, John C.

doi:10.1002/mas.1280140203

Cited by 391 publications

(225 citation statements)

References 112 publications

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“…In addition, these transition-metal containing ions may provide new and complementary fragmentation information when subjected to collision induced dissociation (CID) or other dissociation techniques. Previous studies have shown that ESI can be used to readily form gaseous complex ions composed of a transition-metal and one or more multi-dentate ligands [25][26][27][28]. Such metal complex ions have been the subject of extensive study including CID [29 -33] and ion/molecule reactions [34 -36].…”

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confidence: 99%

Gas-phase ion/ion reactions of transition metal complex cations with multiply charged oligodeoxynucleotide anions

Barlow

Hodges

Xia

et al. 2008

J. Am. Soc. Mass Spectrom.

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Multiply deprotonated hexadeoxyadenylate anions, (A 6 ϪnH) nϪ , where n ϭ 3-5, have been subjected to reaction with a range of divalent transition-metal complex cations in the gas phase. The cations studied included the bis-and tris-1,10-phenanthroline complexes of Cu II , Fe II , and Co II , as well as the tris-1,10-phenanthroline complex of Ru II . In addition, the hexadeoxyadenylate anions were subjected to reaction with the singly charged Fe III and Co III N,N=-ethylenebis(salicylideneiminato) complexes. The major competing reaction channels are electron-transfer from the oligodeoxynucleotide anion to the cation, the formation of a complex between the anion and cation, and the incorporation of the transition-metal into the oligodeoxynucleotide. The latter process proceeds via the anion/cation complex and involves displacement of the ligand(s) in the transition-metal complex by the oligodeoxynucleotide. Competition between the various reaction channels is governed by the identity of the transition-metal cation, the coordination environment of the metal complex, and the oligodeoxynucleotide charge state. In the case of the divalent metal phenanthroline complexes, competition between electron-transfer and metal ion incorporation is particularly sensitive to the coordination number of the reagent metal complexes. Both electron-transfer and metal ion incorporation occur to significant extents with the bis-phenanthroline ions, whereas the trisphenanthroline ions react predominantly by metal ion incorporation. To our knowledge this work reports the first observations of the gas-phase incorporation of multivalent transition-metal cations into oligodeoxynucleotide anions and represents a means for the selective incorporation of transition-metal counter-ions into gaseous oligodeoxynucleotides. [6 -8] have allowed the formation of gas-phase ions of biopolymers, including oligodeoxynucleotides (ODNs), making these ions amenable to study by mass spectrometry. Like peptides and proteins, ODNs are amphoteric, [9] allowing formation of either positively or negatively charged ions. Formation of negatively charged oligonucleotides is quite facile using ESI and, as a result, negatively charged ODN ions have been the most widely studied [9]. Oligodeoxynucleotide ions with bound metals formed by MALDI or ESI, especially those containing transition metals, have shown fragmentation behavior, which is distinct and complementary to that of ions devoid of metals [6 -8].The study of the interaction of transition metals with DNA is of critical importance, given the variety of roles such interactions fulfill. Transition-metal complexes display nuclease activity and consequently complexes such as (methidium-propyl-EDTA)iron(II) have been utilized as footprinting agents [10]. Ruthenium(II) complexes have been extensively examined as spectroscopic probes of local DNA structure [11,12]. The mechanism of action of the chemotherapeutic agent cisplatin involves binding to DNA to prevent replication [13][14][15]. Mass spectrometry has been u...

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confidence: 99%

Gas-phase ion/ion reactions of transition metal complex cations with multiply charged oligodeoxynucleotide anions

Barlow

Hodges

Xia

et al. 2008

J. Am. Soc. Mass Spectrom.

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“…[3][4][5][6][7][8][9][10] On the other hand, because of the complexity of a real sample, the chromatographic separation of the target metallic element species was usually necessary for its speciation. [11][12][13][14][15] In this study, the interaction of lanthanum with ethylenediamine tetraacetic acid (EDTA), which has donor atoms of nitrogen and oxygen, and may be considered as a model ligand existing in the environment, and with Ltryptophen (Try) as the basic unit of a protein, were studied by the cation-exchange HPLC coupled with ESI-MS. The stability of La species during a cation-exchange chromatographic separation process is also discussed in this paper for obtaining accurate information on lanthanum speciation.…”

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confidence: 99%

Evaluation of Dissolved Species of Lanthanum in the Solutions Containing Different Amino Acids by Cation-Exchange Chromatography Coupled with Electrospray Ionization Mass Spectrometry

et al. 2000

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Because the separation and purification methods of rare-earth elements (REEs) are well developed, REEs have recently been widely used in many fields of industry and agriculture. The widespread application of REEs as additives in fertilizers, especially in China, 1 inherently leads to their residues in the environment, accumulation in organisms, and entering into the food chain. Moreover, the bioavailability and toxicity of REEs mainly depend on its dissolved species, which can be partly assimilated by plants and animals. Thus, the speciation analysis of REEs in the environment and organisms is becoming ever more important today. The study of the interaction of REEs with humic substances and proteins is a useful way to understand their behavior in the environment or during the biological process of an organism.Electrospray ionization (ESI), as a soft source for mass spectrometry (MS), has recently been used to evaluate the chemical species of dissolved metal ions; it provides information on the interaction between metal ions and organic ligands, which forms the basis of many essential biochemical processes. [3][4][5][6][7][8][9][10] On the other hand, because of the complexity of a real sample, the chromatographic separation of the target metallic element species was usually necessary for its speciation. [11][12][13][14][15] In this study, the interaction of lanthanum with ethylenediamine tetraacetic acid (EDTA), which has donor atoms of nitrogen and oxygen, and may be considered as a model ligand existing in the environment, and with Ltryptophen (Try) as the basic unit of a protein, were studied by the cation-exchange HPLC coupled with ESI-MS. The stability of La species during a cation-exchange chromatographic separation process is also discussed in this paper for obtaining accurate information on lanthanum speciation. Experimental Reagents and chemicalsLanthanum oxide (La2O3) was obtained from Changchun Institute of Applied Chemistry of the Chinese Academy of Sciences; purity >99.9999%. La stock solution (1.00 mg cm -3 ) was prepared by dissolving an appropriate amount of La2O3, which had been ignited at 850˚C for 4 h, in 2 mol dm -3 HNO3, and then diluted with doubly deionized Milli-Q water to 100 mL in a polyethylene bottle. Ligand stock solutions (5×10 -3 mol dm -3 ) were prepared by dissolving EDTA-Na2 (A. R., Shanghai Reagent Factory) with doubly deionized Milli-Q water, and Try (purity >99%, Shanghai Bo-Ao Bio-Technology Co.) with a 1:1 water-methanol solution in acid-washed polyethylene bottles. HPLC-grade methanol was obtained from Shanghai Wusong Chemical Factory. An ammonium acetate-acetic acid (A. R., Shanghai Reagent Factory) solution (1×10 -3 mol dm -3 , pH 5 -6) was used as a buffer. Formic acid (A. R., Shanghai Reagent Factory) and α-hydroxyisobutyric acid (α-HIBA, Hunan Institute of Rare-earth Metals of China, A. R.) solutions were used as mobile phases for HPLC separation. Samples were prepared by combining the calculated amount of stock and buffer solutions to give an La concentration of 1×10...

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“…Electrospray (ES) ionization [34,35] coupled with tandem MS (MS/MS) has become a powerful tool for analyses of nanoparticle composition [22-24, 30, 36 -38] provided that the nanoparticle can be suspended in a solvent of moderate polarity without decomposition or other reactions. Laser desorption/ionization time-of-flight mass spectrometry (LDI-TOF-MS) has also been used to record mass spectra and determine specific atomic compositions of large gold nanocrystals with masses of tens of kilodaltons without the use of matrices [25][26][27][28].…”

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Characterization of synthesized titanium oxide nanoclusters by MALDI-TOF mass spectrometry

Guan

Lü

Fang

et al. 2007

J. Am. Soc. Mass Spectrom.

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Titania represents an important material that has wide applications. The bactericidal efficiency of TiO 2 has been shown to be dependent on the size of the nanoparticles, so it is important to be able to reliably estimate their dimensions. In this study, a stable TiO 2 cluster suspension is produced by the thermal solvent process, and ultrasmall clusters (Ͻ1 nm) with different sizes are obtained by size-selection treatment. MALDI-TOF-MS and LDI-TOF-MS are shown to be useful for characterization of these ultrasmall nanoparticles. Peak maxima are found to correlate with nanoparticle size, and the possibility of using these mass spectrometry-based approaches to estimate nanoparticle size is affirmed. The size distributions of TiO 2 nanoparticles obtained from MALDI-and LDI-TOF-MS are in good agreement with parallel TEM observations. Finally, PSD analysis of inorganic nanomaterials is performed and valuable information about the structure of analytes has been obtained. (J Am Soc Mass Spectrom 2007, 18, 517-524)

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Electrospray mass spectrometry applied to inorganic and organometallic chemistry

Cited by 391 publications

References 112 publications

Gas-phase ion/ion reactions of transition metal complex cations with multiply charged oligodeoxynucleotide anions

Gas-phase ion/ion reactions of transition metal complex cations with multiply charged oligodeoxynucleotide anions

Evaluation of Dissolved Species of Lanthanum in the Solutions Containing Different Amino Acids by Cation-Exchange Chromatography Coupled with Electrospray Ionization Mass Spectrometry

Characterization of synthesized titanium oxide nanoclusters by MALDI-TOF mass spectrometry

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