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Revisiting Dissolved Organic Matter Analysis Using High-Resolution Trapped Ion Mobility and FT-ICR Mass Spectrometry.

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|September 12, 2024
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Summary
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Analyzing complex mixtures like dissolved organic matter is challenging. This study enhances molecular characterization by optimizing trapped ion mobility separation-Fourier transform ion cyclotron resonance mass spectrometry (TIMS-FT-ICR MS) techniques for greater formula assignment.

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Area of Science:

  • Analytical Chemistry
  • Environmental Chemistry
  • Organic Geochemistry

Background:

  • Characterizing complex mixtures at the molecular level is a significant analytical hurdle.
  • High-resolution gas-phase separations offer potential for detailed isomeric content description.

Purpose of the Study:

  • To evaluate the analytical capabilities of trapped ion mobility separation coupled with Fourier transform ion cyclotron resonance mass spectrometry (TIMS-FT-ICR MS) for dissolved organic matter (DOM) analysis.
  • To investigate the impact of data acquisition systems, processing strategies, ICR cell geometries, and magnetic field strengths on DOM characterization.

Main Methods:

  • Utilized high-resolution TIMS coupled with FT-ICR MS for analyzing a Harney River DOM sample.
  • Compared TIMS-MS separation capabilities against MS alone.
  • Evaluated external high-performance data acquisition (DAQ) systems, including absorption mode FT (aFT) versus magnitude mode FT (mFT).
  • Assessed the effects of apodization windows (half vs. full) and varying magnetic field strengths (7 T, 9.4 T, 21 T).

Main Results:

  • External high-performance DAQ with aFT processing doubled MS resolution compared to default mFT.
  • Employing half-apodization (Kaiser-type) and aFT increased assigned formulas by 45% for DOM analysis.
  • Reprocessing 2D-TIMS-FT-ICR MS data with higher resolving power and magnetic field strength (21 T) led to a 24% increase in reported isomers.

Conclusions:

  • Optimized TIMS-FT-ICR MS parameters, including advanced DAQ and higher magnetic fields, significantly enhance the molecular-level characterization of complex DOM.
  • The integration of complementary separation techniques and advanced data processing strategies is crucial for detailed isomeric content description in complex mixtures.