Non-targeted analysis, interactive visualization, and online sharing of interactive LC-HRMS/MS data of polymers using a comprehensive software PolyMatch Suite

Význam tématu

Polymers and oligomeric series play a vital role in everyday materials such as plastics, excipients, emulsifiers, lubricants, and detergents. However, these compounds can also act as contaminants or spectral interferences that complicate non-targeted liquid chromatography–high-resolution mass spectrometry (LC-HRMS) analyses. Effective identification and annotation of polymeric species are therefore essential for quality control, environmental monitoring, and product development.

Cíle a přehled studie / článku

This study demonstrates the capabilities of PolyMatch Suite, an open-source software platform designed for comprehensive polymer discovery and non-targeted analysis. The primary goals are to illustrate (1) the development of extensive polymer and oligomer libraries, (2) an automated end-to-end data processing workflow, and (3) an interactive visualization interface with web-based sharing to accelerate annotation and decision-making.

Použitá metodika a instrumentace

Data Acquisition and Instrumentation:

• Agilent 6546 LC/Q-TOF system operated in full-scan, data-dependent acquisition (DDA), and iterative exclusion DDA (IE-DDA) modes.
• Blank and pooled sample injections to support background filtering.

Software Workflow:

• File conversion and peak picking via vendor tools or open-source packages (e.g., MZMine 4).
• Automated blank filtration and feature grouping based on mass defect and chromatographic retention time.
• Compound annotation using the PolyMatch Flow or modular Python scripts, leveraging class-based libraries and fragmentation rules.
• Interactive visualization employing PolyVI for cross-filtered plots (mass defect, retention time vs. m/z, MS/MS spectra, extracted ion chromatograms).

Library Composition:

• Over 775,000 unique polymeric species including polysorbate, polysorbide, and polyethylene glycol (PEG) variants, with associated SMILES, formulas, and fragmentation rules.
• Dedicated sub-libraries for fatty acid esters and novel adduct forms.
• Custom library generation via PolyMatch Generator for user-defined homologous series.

Hlavní výsledky a diskuse

Library Coverage and Annotation Performance:

• Successful identification of Polysorbate 80 components, ranging from PEG-8 to PEG-12 and C18:1 fatty acid esters.
• Low false positive rate (<5%) achieved through combined use of mass defect filtering, retention time trends, exact mass matches, and MS/MS fragmentation evidence.
• Annotation of over 150,000 species with detailed fragmentation screening and substructure assignment capabilities.

Visualization and Validation:

• Mass defect plots normalized to repeating units enable rapid class discrimination.
• Retention time vs. m/z series plots highlight homologous polymer distributions.
• Dynamic cross-filtering across all MS evidences allows simultaneous inspection of MS1, MS/MS, and chromatographic traces.
• Web-shareable links facilitate collaborative review without requiring software installation.

Přínosy a praktické využití metody

PolyMatch Suite streamlines the non-targeted analysis of complex polymer mixtures by automating raw data processing, annotation, and interactive visualization. Key benefits include:

• Rapid and reproducible polymer annotation in environmental, pharmaceutical, and materials science contexts.
• Discovery of previously unreported oligomeric species and contaminants.
• Customizable libraries and workflows accommodate novel polymer chemistries and user-specific research needs.
• Enhanced communication through interactive visual reports and weblink sharing.

Budoucí trendy a možnosti využití

Emerging directions for PolyMatch and non-targeted polymer analysis encompass:

• Integration with data-independent acquisition (DIA) strategies and tandem MS platforms for deeper structural insights.
• Expansion of community-driven libraries and fragmentation rule sets to cover new polymer classes.
• Cloud-based and collaborative environments enabling real-time sharing and annotation across distributed teams.
• Machine learning-based scoring algorithms to refine annotation confidence and reduce manual validation efforts.

Závěr

PolyMatch Suite offers a robust, user-friendly solution for the comprehensive, non-targeted analysis of polymers and oligomers. By combining large curated libraries, automated workflows, and interactive visual tools, the platform significantly enhances the speed, accuracy, and transparency of polymer identification in complex LC-HRMS datasets.

Reference

Koelmel J; Weil DA; Rennie EE; Stelben P; Oranzi N; Kummer M; Godri D; Qi J; Lin EZ; Godri Pollitt KJ. Non-targeted analysis, interactive visualization, and online sharing of interactive LC-HRMS/MS data of polymers using PolyMatch Suite. ASMS 2024, MP 216.