Dataset Information

Sequencing of Side-Chain Liquid Crystalline Copolymers by Matrix-Assisted Laser Desorption/Ionization Tandem Mass Spectrometry.

ABSTRACT: Polyether based side-chain liquid crystalline (SCLC) copolymers with distinct microstructures were prepared using living anionic polymerization techniques. The composition, end groups, purity, and sequence of the resulting copolymers were elucidated by matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) and tandem mass spectrometry (MS/MS). MALDI-MS analysis confirmed the presence of (CH3)3CO- and -H end groups at the initiating (?) and terminating (?) chain end, respectively, and allowed determination of the molecular weight distribution and comonomer content of the copolymers. The comonomer positions along the polymer chain were identified by MS/MS, from the fragments formed via C-O and C-C bond cleavages in the polyether backbone. Random and block architectures could readily be distinguished by the contiguous fragment series formed in these reactions. Notably, backbone C-C bond scission was promoted by a radical formed via initial C-O bond cleavage in the mesogenic side chain. This result documents the ability of a properly substituted side chain to induce sequence indicative bond cleavages in the polyether backbone.

SUBMITTER: Snyder SR

PROVIDER: S-EPMC6680698 | biostudies-literature | 2019 Jul

REPOSITORIES: biostudies-literature

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Sequencing of Side-Chain Liquid Crystalline Copolymers by Matrix-Assisted Laser Desorption/Ionization Tandem Mass Spectrometry.

Snyder Savannah R SR Wei Wei W Xiong Huiming H Wesdemiotis Chrys C

Polymers 20190701 7

Polyether based side-chain liquid crystalline (SCLC) copolymers with distinct microstructures were prepared using living anionic polymerization techniques. The composition, end groups, purity, and sequence of the resulting copolymers were elucidated by matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) and tandem mass spectrometry (MS/MS). MALDI-MS analysis confirmed the presence of (CH<sub>3</sub>)<sub>3</sub>CO- and -H end groups at the initiating (α) and terminating (ω) ...[more]

PMID: 31266225

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Project description:A liquid matrix-assisted laser desorption/ionization (liquid MALDI) method has been developed for high-throughput atmospheric pressure (AP) mass spectrometry (MS) analysis of the molecular content of crude bioliquids for disease diagnostics. The presented method is rapid and highly robust, enabling its application in environments where speed and low-cost high-throughput analyses are required. Importantly, because of the creation of multiply charged analyte ions, it provides additional functionalities that conventional solid MALDI MS profiling is lacking, including the use of high-performance mass analyzers with limited m/z range. The concomitant superior MS/MS performance that is achieved similar to ESI MS/MS adds greater analytical power and specificity to MALDI MS profiling while retaining the advantages of a fast laser-based analysis system and off-line large-scale sample preparation. The potential of this MALDI MS profiling method is demonstrated on the detection of dairy cow mastitis, which is a substantial economic burden on the dairy industry with losses of hundreds of dollars per diseased cow per year, equating to a total annual loss of billions of dollars, as well as leading to the use of large quantities of antibiotics, adding to the proliferation of antimicrobial resistance. Only small amounts of aliquots obtained from the daily farm milking process were prepared for liquid MALDI MS profiling using a simple one-pot/two-step analyte extraction. Automated analysis was performed using a custom-built AP-MALDI ion source, enabling the simultaneous detection of lipids, peptides, and proteins. Diagnostic, multiply charged, proteinaceous ions were easily sequenced and identified by MS/MS experiments. Samples were classified according to mastitis status using multivariate analysis, achieving 98.5% accuracy (100% specificity) determined by "leave 20% out" cross-validation. The methodology is generally applicable to AP-MALDI MS profiling on most commercial high-resolution mass spectrometers, with the potential for expansion into hospitals for rapid assessment of human and other biofluids.

Dataset Information

Sequencing of Side-Chain Liquid Crystalline Copolymers by Matrix-Assisted Laser Desorption/Ionization Tandem Mass Spectrometry.

Publications

Sequencing of Side-Chain Liquid Crystalline Copolymers by Matrix-Assisted Laser Desorption/Ionization Tandem Mass Spectrometry.

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