Enhancing carbohydrate ion yield by controlling crystalline structures in matrix-assisted laser desorption/ionization mass spectrometry

Lee, Hsun; Lai, Yin‐Hung; Ou, Yumeng; Tsao, Chien-Wei; Jheng, Ya-Jin; Kuo, Shu-Yun; Wang, Yi-Sheng

doi:10.1016/j.aca.2017.09.024

Cited by 8 publications

(11 citation statements)

References 28 publications

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“…However, the observation showed in Figure S1 is a case prepared by using 3‐μL mixture of globo H and DHB. Sample heterogeneity problem can be effectively reduced by changing sample preparation protocols . Table S1 summarizes the surface quality obtained by using 0.1 and 1 μL of the same mixture or the mixture of globo H and α ‐cyano‐4‐hydroxycinnamic acid matrix.…”

Section: Resultsmentioning

confidence: 99%

“…Sample heterogeneity problem can be effectively reduced by changing sample preparation protocols. 31 Table S1 summarizes the surface quality obtained by using 0.1 and 1 μL of the same mixture or the mixture of globo H and α-cyano-4-hydroxycinnamic acid matrix. The data indicate that reduced surface roughness (mean deviation) can be readily achieved using smaller amount of sample.…”

Section: Contributions Of Initial Velocity Spread and Sample Thicknessmentioning

confidence: 99%

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Impact of uneven sample morphology on mass resolving power in linear MALDI‐TOF mass spectrometry: A comprehensive theoretical investigation

Cai

Wang

2018

J Mass Spectrom

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This work discusses the correlation between the mass resolving power of matrix-assisted laser desorption/ionization time-of-flight mass analyzers and extraction condition with an uneven sample morphology. Previous theoretical calculations show that the optimum extraction condition for flat samples involves an ideal ion source design and extraction delay. A general expression of spectral feature takes into account ion initial velocity, and extraction delay is derived in the current study. The new expression extends the comprehensive calculation to uneven sample surfaces and above 90% Maxell-Boltzmann initial velocity distribution of ions to account for imperfect ionization condition. Calculation shows that the impact of uneven sample surface or initial spatial spread of ions is negligible when the extraction delay is away from the ideal value. When the extraction delay approaches the optimum value, the flight-time topology shows a characteristic curve shape, and the time-domain mass spectral feature broadens with an increase in initial spatial spread of ions. For protonated 2,5-dihydroxybenzoic acid, the mass resolving power obtained from a sample of 3-μm surface roughness is approximately 3.3 times lower than that of flat samples. For ions of m/z 3000 coexpanded with 2,5-dihydroxybenzoic acid, the mass resolving power in the 3-μm surface roughness case only reduces roughly 7%. Comprehensive calculations also show that the mass resolving power of lighter ions is more sensitive to the accuracy of the extraction delay than heavier ions.

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Section: Resultsmentioning

confidence: 99%

Section: Contributions Of Initial Velocity Spread and Sample Thicknessmentioning

confidence: 99%

Impact of uneven sample morphology on mass resolving power in linear MALDI‐TOF mass spectrometry: A comprehensive theoretical investigation

Cai

Wang

2018

J Mass Spectrom

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“…, for example, have re-examined the optimal concentration of NaCl added to a target of ovalbumin glycans and DHB and found that concentrations of 0.01-0.1 M are optimal, with results being obtained on two TOF instruments. Small crystals, induced by vacuum drying or recrystallization from methanol (Lee, Lai, et al, 2017; F I G U R E 1 ATDs of the fragment ions at m/z 1558 ( 2,4 A 6 ) from three isomers of the high-mannose N-glycan, Man 8 GlcNAc 2 .…”

Section: Common Matricesmentioning

confidence: 99%

“…Kim, Shin, et al (2017), for example, have re‐examined the optimal concentration of NaCl added to a target of ovalbumin glycans and DHB and found that concentrations of 0.01–0.1 M are optimal, with results being obtained on two TOF instruments. Small crystals, induced by vacuum drying or recrystallization from methanol (Lee, Lai, et al, 2017; Ou, Kuo, et al, 2018) or ethanol (Harvey, 1993) have been shown to greatly improve ion signal strength by reducing crystal size. Practical details of the methanol recrystallization method used by Ou, Kuo, et al (2018) have been made into a video.…”

Section: Matricesmentioning

confidence: 99%

Analysis of carbohydrates and glycoconjugates by matrix‐assisted laser desorption/ionization mass spectrometry: An update for 2017–2018

Harvey

2021

Mass Spectrometry Reviews

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This review is the tenth update of the original article published in 1999 on the application of matrix‐assisted laser desorption/ionization mass spectrometry (MALDI) mass spectrometry to the analysis of carbohydrates and glycoconjugates and brings coverage of the literature to the end of 2018. Also included are papers that describe methods appropriate to glycan and glycoprotein analysis by MALDI, such as sample preparation techniques, even though the ionization method is not MALDI. Topics covered in the first part of the review include general aspects such as theory of the MALDI process, new methods, matrices, derivatization, MALDI imaging, fragmentation and the use of arrays. The second part of the review is devoted to applications to various structural types such as oligo‐ and poly‐saccharides, glycoproteins, glycolipids, glycosides, and biopharmaceuticals. Most of the applications are presented in tabular form. The third part of the review covers medical and industrial applications of the technique, studies of enzyme reactions, and applications to chemical synthesis. The reported work shows increasing use of combined new techniques such as ion mobility and highlights the impact that MALDI imaging is having across a range of diciplines. MALDI is still an ideal technique for carbohydrate analysis and advancements in the technique and the range of applications continue steady progress.

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“…However, spatial resolution is dependent on matrix crystal size and laser spot size, 14 which can be optimized to achieve required sensitivity by depositing well‐incorporated, small, homogeneous matrix–analyte co‐crystals 14,15 . Several groups have demonstrated that mixing multiple matrices along with recrystallization improves crystal morphology 16,17 . Even though spatial resolution of 10 μm has been demonstrated in lipid imaging of cancerous tissues, there can be significant challenges associated with sample preparation, which leads to low ion abundance and ultimately poor ion image quality 13,18 .…”

Section: Introductionmentioning

confidence: 99%

Single‐filament imaging mass spectrometry lipidomics in Arthrospira platensis

Lesco

Rowland

Williams

et al. 2023

Rapid Comm Mass Spectrometry

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Rationale: Elucidating intra-organismal biochemical and lipid organization in photosynthetic biological cell factories of filamentous cyanobacteria, such as Arthrospira platensis (Spirulina), is important for tracking physiological response mechanisms during growth. Little is known about the filaments' biochemical organization and cellular structure and no label-free imaging techniques exist that provide molecular mapping.Methods: We applied ultrahigh-resolution mass spectrometry (MS) with matrixassisted laser desorption ionization (MALDI) imaging to immobilized Spirulina filaments to investigate the localization of lipids across distinct physiological regions.We optimized matrix selection and deposition methods with the goal of facilitating high spatial, and intra-filament, resolution using untargeted multivariate statistical spectral deconvolution across MS pixels.Results: Our results demonstrate an improved two-step matrix application with an optimized procedure for intra-organismal lipid profiling to improve analyte sensitivity and achieve higher spatial resolution. We evaluate several conventional matrices, namely 2,5-dihydroxybenzoic acid (DHB), superDHB (sDHB), 1,5-diaminonaphthalene (DAN), and a 50:50 mix of DHB and sDHB, and compare delineation and pixel-based elucidation of intra-filament lipidomics. We identified a total of 1626 features that could be putatively assigned a lipid-like formula based on database query and 46 unique features, with associated lipid assignments that were significantly distinct in their intra-filament location.Conclusions: MALDI imaging MS with untargeted statistical spectral deconvolution was used to visualize intra-filament lipidomics organization in Spirulina filaments.Improvements in matrix deposition, including sequential sublimation and pneumatic spraying, increased signal abundance at high spatial resolution and allowed for identification of distinct lipid composition regions. This work outlines a methodology that may be used for micro-ecological untargeted molecular phenotyping.

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Enhancing carbohydrate ion yield by controlling crystalline structures in matrix-assisted laser desorption/ionization mass spectrometry

Cited by 8 publications

References 28 publications

Impact of uneven sample morphology on mass resolving power in linear MALDI‐TOF mass spectrometry: A comprehensive theoretical investigation

Impact of uneven sample morphology on mass resolving power in linear MALDI‐TOF mass spectrometry: A comprehensive theoretical investigation

Analysis of carbohydrates and glycoconjugates by matrix‐assisted laser desorption/ionization mass spectrometry: An update for 2017–2018

Single‐filament imaging mass spectrometry lipidomics in Arthrospira platensis

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