Solid-state NMR spectroscopy as a tool supporting optimization of MALDI-TOF MS analysis of polylactides

Sroka-Bartnicka, Anna; Olejniczak, Sebastian; Sochacki, Marek; Biela, Tadeusz; Potrzebowski, Marek J.

doi:10.1016/j.jasms.2008.09.013

Cited by 10 publications

(8 citation statements)

References 24 publications

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“…The characterization of solid‐state structures at the atomic level can also be performed using solid‐state nuclear magnetic resonance (NMR), which can reveal differences between samples that look identical when analyzed by other solid‐state techniques. However, only a few reported studies have used solid‐state NMR to scrutinize molecular organization in MALDI samples 39–42 . NMR can explore various morphological systems, such as those obtained for MALDI samples, as a function of crystallization conditions 40 .…”

Section: Introductionmentioning

confidence: 99%

“…However, only a few reported studies have used solid-state NMR to scrutinize molecular organization in MALDI samples. [39][40][41][42] NMR can explore various morphological systems, such as those obtained for MALDI samples, as a function of crystallization conditions. 40 NMR data permitted us to show that mechano-induced reactions occurred on grinding the matrix (2,5-DHB) together with the salt (CsF) to prepare a solid binary mixture for MALDI of PEG; strong interactions between the matrix and the cation led to the formation of a salt in the presence of some water molecules.…”

Section: Introductionmentioning

confidence: 99%

“…[39][40][41][42] NMR can explore various morphological systems, such as those obtained for MALDI samples, as a function of crystallization conditions. 40 NMR data permitted us to show that mechano-induced reactions occurred on grinding the matrix (2,5-DHB) together with the salt (CsF) to prepare a solid binary mixture for MALDI of PEG; strong interactions between the matrix and the cation led to the formation of a salt in the presence of some water molecules. 39 Moreover, an NMR study of 2,5-DHB/PEG/CsCl ternary mixtures allowed three main matrix phases to be identified as a function of the grinding time, and different MALDI activity was measured for each phase.…”

Section: Introductionmentioning

confidence: 99%

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Using solid‐state nuclear magnetic resonance to rationalize best efficiency of 2,6‐dihydroxybenzoic acid over other 2,X‐dihydroxybenzoic acid isomers in solvent‐free matrix‐assisted laser desorption/ionization of poly(ethylene glycol)

Pizzala

Chendo

Charles

2020

Rapid Comm Mass Spectrometry

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RationaleAmong isomers of dihydroxybenzoic acid (DHB), 2,5‐DHB is often the most efficient matrix in matrix‐assisted laser desorption/ionization mass spectrometry (MALDI‐MS) for a great variety of compounds. Yet, when performing solvent‐free MALDI, 2,6‐DHB yields better results for poly(ethylene glycol [PEG]). This intriguing feature is explored here using solid‐state nuclear magnetic resonance (NMR).MethodsTernary mixtures were prepared by grinding 2,X‐DHB (X = 3–6), poly(ethylene glycol) (Mn = 2000 g mol−1) and lithium fluoride (LiF) in a matrix/analyte/salt molar ratio of 50/1/10 for 16 min under a controlled atmosphere. After mixing, a few grains were applied to the MALDI target for MS analysis, whereas the major part of the ground sample was transferred into rotors to perform 13C, 7Li, and 19F NMR experiments.ResultsLithiated PEG chains are mainly formed with 2,6‐DHB in solvent‐free MALDI, but their abundance increases with 2,3‐DHB and 2,4‐DHB when water uptake is favored by a humid atmosphere. Solid‐state NMR shows that grinding 2,6‐DHB‐based samples in atmospheric conditions leads to a solid phase in which the matrix, PEG, and salt molecules exhibit a high mobility compared with systems involving other 2,X‐DHB isomers. This mobile environment would favor (as a solvent) LiF dissociation and best promote PEG cationization.ConclusionsComplementary data in 13C, 7Li, and 19F NMR spectra are consistent with the formation of a solid phase of high mobility composed of 2,6‐DHB, PEG, and the two salt components that ultimately favor the production of lithiated PEG chains.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Using solid‐state nuclear magnetic resonance to rationalize best efficiency of 2,6‐dihydroxybenzoic acid over other 2,X‐dihydroxybenzoic acid isomers in solvent‐free matrix‐assisted laser desorption/ionization of poly(ethylene glycol)

Pizzala

Chendo

Charles

2020

Rapid Comm Mass Spectrometry

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“…Although amorphous materials spectra tend to display broader lines than polycrystalline powder, NMR is able to explore various morphological systems. In particular, the use of solid-state NMR was very recently reported to test the influence of crystallization conditions on MALDI sample morphology [22]. Moreover, a main advantage of this technique is its ability to access many different nuclides, so that data from different elements in a given sample provide complementary information.…”

mentioning

confidence: 99%

Solid state nuclear magnetic resonance as a tool to explore solvent-free MALDI samples

Pizzala

Barrère

Mazarin

et al. 2009

J. Am. Soc. Mass Spectrom.

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Solid-state Nuclear magnetic resonance (NMR) was used here to explore structural characteristics of samples to be subjected to matrix-assisted laser desorption/ionization (MALDI) and prepared without the use of any solvent. The analytical systems scrutinized in NMR were mixtures of a 2,5-dihydroxybenzoic acid (2,5-DHB) matrix and caesium fluoride (CsF), used as the cationization agent in synthetic polymer MALDI mass analysis, at different molar ratios (1:1, 5:1, and 10:1). Complementary information could be obtained from 13 C, 133 Cs, and 19 F NMR spectra. Grinding the matrix together with the salt in the solid state was shown to induce a strong modification in the molecular organization within the MALDI sample. The evidenced mechano-induced reactions allow strong interactions between the matrix and the cation, up to the formation of a salt, and only occur in the presence of some water molecules. Addition of a poly(ethylene oxide) polymer as the analyte did not further modify the observed molecular organizations. Although relative matrix and salt concentrations in the scrutinized samples were unusual for MALDI analysis, mass spectra of good quality could be obtained and revealed that cation attachment on polymers during the MALDI process is not a matrix-independent event since a lower ionization efficiency was obtained from highly organized solid samples, mostly consisting of 2,5-DHB caesium salt species. (J Am Soc Mass Spectrom 2009, 20, 1906 -1911) © 2009 American Society for Mass Spectrometry M atrix-assisted laser desorption/ionization (MALDI) is widely used as an efficient ionization method to characterize synthetic polymers by time-of-flight mass spectrometry (TOF MS) [1,2]. A key point in the success of a MALDI-MS analysis is sample preparation, that is, proper matrix and cation selection as well as solid-state organization. The matrix actually plays multiple roles in the MALDI process and should accordingly present specific properties. Some criteria are clearly defined, such as a strong absorptivity at the employed laser wavelength or good vacuum stability, while other requirements, such as a good miscibility of the matrix with the analyte in the solid state, are not easily related to physico-chemical parameters of the matrix. As a result, prediction for the optimal matrix-polymer system is still not possible and sample preparation methods are usually developed from published protocols that were shown to work for a given polymeric system [3]. In particular, solvent-free MALDI was recently proposed as an alternative to the conventional dried droplet method [4,5].Despite MALDI being a widely used technique, mechanisms underlying this desorption/ionization process are still not fully understood. To investigate the MALDI process, many studies have focused on sample morphology using different imaging experiments. Sample heterogeneity and distribution of molecules within the MALDI solid sample have been explored using microscopy techniques, such as optical microscopy [6,7], scanning electron microscopy [8 -...

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“…Co-crystallization of the target analyte and polymorphism of the MALDI matrix can be studied using several techniques: e.g., solid-state NMR [ 35 , 36 ], Raman imaging [ 37 , 38 ], confocal fluorescence microscopic imaging [ 39 ], and MS imaging [ 40 , 41 ]. Moreover, a variety of other techniques can determine the homogeneity of the crystals and the effectiveness of the desorption and ionization processes [ 42 ].…”

Section: Resultsmentioning

confidence: 99%

N-Glycan profile analysis of transferrin using a microfluidic compact disc and MALDI-MS

et al. 2016

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It has been known for a long time that diseases can be associated with changes to the glycosylation of specific proteins. This has been shown for cancer, immunological disorders, and neurodegenerative diseases. The possibility of using the glycosylation patterns of proteins as biomarkers for disease would be a great asset for clinical research or diagnosis. There is at present a lack of rapid, automated, and cost-efficient analytical techniques for the determination of the glycosylation of specific serum proteins. We have developed a method for determining the glycosylation pattern of proteins based on the affinity capture of a specific serum protein, the enzymatic release of the N-linked glycans, and the analysis of the glycan pattern using MALDI-MS. All sample preparation is performed in a disposable centrifugal microfluidic disc. The sample preparation is miniaturized, requiring only 1 μL of sample per determination, and automated with the possibility of processing 54 samples in parallel in 3.5 h. We have developed a method for the glycosylation pattern analysis of transferrin. The method has been tested on serum samples from chronic alcohol abusers and a control group. Also, a SIMCA model was created and evaluated to discriminate between the two groups.

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Solid-state NMR spectroscopy as a tool supporting optimization of MALDI-TOF MS analysis of polylactides

Cited by 10 publications

References 24 publications

Using solid‐state nuclear magnetic resonance to rationalize best efficiency of 2,6‐dihydroxybenzoic acid over other 2,X‐dihydroxybenzoic acid isomers in solvent‐free matrix‐assisted laser desorption/ionization of poly(ethylene glycol)

Using solid‐state nuclear magnetic resonance to rationalize best efficiency of 2,6‐dihydroxybenzoic acid over other 2,X‐dihydroxybenzoic acid isomers in solvent‐free matrix‐assisted laser desorption/ionization of poly(ethylene glycol)

Solid state nuclear magnetic resonance as a tool to explore solvent-free MALDI samples

N-Glycan profile analysis of transferrin using a microfluidic compact disc and MALDI-MS

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