Simple Pretreatment for the Analysis of Additives and Polymers by Surface-Assisted Laser Desorption/Ionization Mass Spectrometry Using a Through-Hole Alumina Membrane as a Functional Substrate

Sato, Hiroaki; Nakamura, Sayaka; Fouquet, Thierry; Ohmura, Takayuki; Kotani, Masahiro; Naito, Yasuhide

doi:10.1021/jasms.9b00048

Cited by 8 publications

(8 citation statements)

References 37 publications

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“…Despite the mechanism being not well defined, a variety of materials such as carbon [ 17 , 19 , 20 ], silicon [ 21 , 22 ], metals [ 23 , 24 , 25 , 26 ], or organic surface coatings [ 27 ] with different nanostructures have also been tested for imaging applications. Among such materials, DIUTHAME (Desorption Ionization Using Through-Hole Alumina Membrane) is showing promising features for an easy and reproducible sample preparation [ 28 , 29 , 30 , 31 ]. DIUTHAME consists of a 5 µm thin alumina membrane, nanostructured with 200 nm through holes.…”

Section: Introductionmentioning

confidence: 99%

Matrix-Free High-Resolution Atmospheric-Pressure SALDI Mass Spectrometry Imaging of Biological Samples Using Nanostructured DIUTHAME Membranes

2021

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Applications of mass spectrometry imaging (MSI), especially matrix-assisted laser desorption/ionization (MALDI) in the life sciences are becoming increasingly focused on single cell analysis. With the latest instrumental developments, pixel sizes in the micrometer range can be obtained, leading to challenges in matrix application, where imperfections or inhomogeneities in the matrix layer can lead to misinterpretation of MS images. Thereby, the application of premanufactured, homogeneous ionization-assisting devices is a promising approach. Tissue sections were investigated using a matrix-free imaging technique (Desorption Ionization Using Through-Hole Alumina Membrane, DIUTHAME) based on premanufactured nanostructured membranes to be deposited on top of a tissue section, in comparison to the spray-coating of an organic matrix in a MALDI MSI approach. Atmospheric pressure MALDI MSI ion sources were coupled to orbital trapping mass spectrometers. MS signals obtained by the different ionization techniques were annotated using accurate-mass-based database research. Compared to MALDI MSI, DIUTHAME MS images captivated with higher signal homogeneities, higher contrast and reduced background signals, while signal intensities were reduced by about one order of magnitude, independent of analyte class. DIUTHAME membranes, being applicable only on tissue sections thicker than 50 µm, were successfully used for mammal, insect and plant tissue with a high lateral resolution down to 5 µm.

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Section: Introductionmentioning

confidence: 99%

Matrix-Free High-Resolution Atmospheric-Pressure SALDI Mass Spectrometry Imaging of Biological Samples Using Nanostructured DIUTHAME Membranes

2021

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“…Evaluation tests using liquid samples have confirmed that DIUTHAME has no spot-to-spot fluctuations of signal intensities like MALDI, and as a result, mass spectra with high reproducibility can be acquired. DIUTHAME demonstrates the excellent performance in the analysis of industrial materials and provides the possibilities of simple and rapid analyses of polymer additive molecules and polymer structure analyses based on fragmentation patterns similar to high-energy collision induced dissociation (HE-CID) obtained from polymers. − In addition, DIUTHAME has proved to be suitable for mass spectrometry imaging from an evaluation test using frozen tissue section samples …”

Section: Introductionmentioning

confidence: 99%

Feasibility of Acetylcholinesterase Reaction Assay Monitoring in DIUTHAME-MS

Naito

Kotani

Ohmura

2020

J. Am. Soc. Mass Spectrom.

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DIUTHAME (desorption ionization using through hole alumina membrane) is a novel matrix-free laser desorption/ ionization method that enables highly reproducible acquisition of mass spectra. This study aims to evaluate the applicability of DIUTHAME to the acetylcholinesterase reaction assay (AChE assay) commonly used in high-throughput screening (HTS) in the drug discovery process. The commercially available 9-ch DIUTHAME chip was applied to a series of AChE assays prepared with different reaction times. Numerous positive-mode TOF mass spectra were acquired from the raster-scanned sample spots of the AChE assays to analyze the progress of the enzyme reaction and to perform mass spectrometry imaging of the sample spots. The reaction kinetics plots obtained by DIUTHAME were found to reflect the time course of reaction progression as much as those obtained by MALDI and were found to have less error variation than MALDI. DIUTHAME allowed the already irradiated sample spots to be reused to reproduce the reaction kinetics plots by the second measurement conducted a week after, whereas MALDI was not able to properly reproduce the kinetics plots by remeasuring the irradiated sample spots. In DIUTHAME, which does not require a matrix, the experimental procedure for measuring AChE assay becomes extremely simple. DIUTHAME is potentially able to provide more precise AChE reaction kinetics plots than what have been accomplished by MALDI.

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“…DIUTHAME chip, a novel SALDI technique developed by our group, has shown the capability of MS analyses 46,55–57 and MSI analyses 47,48,58 of lipids in biological tissue sections. In this study, we examined the effect of DIUTHAME on the reproducibility of mass accuracies and intensities by analyzing a standard lipid as well as mouse brain tissue sections.…”

Section: Discussionmentioning

confidence: 99%

Desorption ionization using through‐hole alumina membrane offers higher reproducibility than 2,5‐dihydroxybenzoic acid, a widely used matrix in Fourier transform ion cyclotron resonance mass spectrometry imaging analysis

Hasan

Eto

Mamun

et al. 2021

Rapid Comm Mass Spectrometry

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Rationale DIUTHAME (desorption ionization using through‐hole alumina membrane), a recently developed matrix‐free ionization‐assisting substrate, was examined for reproducibility in terms of mass accuracy and intensity using standard lipid and mouse brain sections. The impregnation property of DIUTHAME significantly improved the reproducibility of mass accuracy and intensity compared with 2,5‐dihydroxybenzoic acid (DHB). Methods Frozen tissue sections were mounted on indium tin oxide‐coated glass slides. DIUTHAME and DHB were applied to individual sections. Subsequently, a solution of a phosphatidylcholine standard, PC(18:2/18:2), was poured onto the DIUTHAME and matrix. Finally, the samples were subjected to laser desorption ionization coupled with Fourier transform ion cyclotron resonance mass spectrometry. The reproducibility was tested by calculating the mean ± standard deviation values of mass errors and intensities of individual ion species. Results Analysis of the PC(18:2/18:2) standard showed significantly (p < 0.01) lower mass error for DIUTHAME‐MS than for MALDI‐MS. Endogenous PC(36:4) analysis in mouse brain section also showed significantly (p < 0.05) lower mass errors for DIUTHAME‐MS. Furthermore, we investigated the mass error of some abundant lipid ions in brain sections and observed similar results. DIUTHAME‐MS displayed lower signal intensity in standard PC analysis. Interestingly, it offered higher signal intensities for all the endogenous lipid ions. Lower fluctuations of both mass accuracies and signal intensities were observed in DIUTHAME‐MS. Conclusions Our results demonstrated that DIUTHAME‐MS offers higher reproducibility for mass accuracies and intensities than MALDI‐MS in both standard lipid and mouse brain tissue analyses. It can potentially be used instead of conventional MALDI‐MS and mass spectrometry imaging analyses to achieve highly reproducible data for mass accuracy and intensity.

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Simple Pretreatment for the Analysis of Additives and Polymers by Surface-Assisted Laser Desorption/Ionization Mass Spectrometry Using a Through-Hole Alumina Membrane as a Functional Substrate

Cited by 8 publications

References 37 publications

Matrix-Free High-Resolution Atmospheric-Pressure SALDI Mass Spectrometry Imaging of Biological Samples Using Nanostructured DIUTHAME Membranes

Matrix-Free High-Resolution Atmospheric-Pressure SALDI Mass Spectrometry Imaging of Biological Samples Using Nanostructured DIUTHAME Membranes

Feasibility of Acetylcholinesterase Reaction Assay Monitoring in DIUTHAME-MS

Desorption ionization using through‐hole alumina membrane offers higher reproducibility than 2,5‐dihydroxybenzoic acid, a widely used matrix in Fourier transform ion cyclotron resonance mass spectrometry imaging analysis

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