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Is high resolution a strict requirement for mass spectrometry-based cellular DNA adductomics?
Yuan-Jhe Chang1, Marcus S Cooke2, Yet-Ran Chen3
1Department of Occupational Safety and Health, Chung Shan Medical University, Taichung, 402, Taiwan; Department of Medical Research, Chung Shan Medical University Hospital, Taichung, 402, Taiwan.
Chemosphere
|May 13, 2021
Summary
DNA adductomics, a tool for exposomics, can now be performed using accessible triple-quadrupole mass spectrometry (QqQ-MS) with statistical analysis. This method shows comparable performance to high-resolution mass spectrometry (HRMS) for pre-screening DNA adducts.
Area of Science:
- Environmental Sciences
- Analytical Chemistry
- Molecular Biology
Background:
- DNA adducts, formed by endogenous and exogenous factors, are linked to gene mutations and cancer development.
- DNA adductomics is a crucial tool for exposomics, aiming to comprehensively detect DNA adducts.
- Liquid chromatography-high resolution mass spectrometry (LC-HRMS) is the current standard for DNA adductomics but is limited by high costs.
Purpose of the Study:
- To compare the analytical performance of high-resolution mass spectrometry (HRMS) with the more accessible triple-quadrupole mass spectrometry (QqQ-MS) for DNA adductomics.
- To evaluate the utility of LC-QqQ-MS coupled with statistical analysis for detecting formaldehyde-induced DNA adducts.
Main Methods:
- Development and optimization of a hybrid quadrupole-linear ion trap-orbitrap MS (Q-LIT-OT-MS) method for detecting purine and pyrimidine adducts.
- Non-targeted screening of formaldehyde-induced DNA adducts using both LC-Q-LIT-OT-MS and LC-QqQ-MS.
- Application of partial least squares-discriminant analysis (PLS-DA) for discriminating false-positive results from QqQ-MS data.
Main Results:
- QqQ-MS successfully detected 12 out of 18 formaldehyde-induced DNA adducts/inter-strand crosslinks (ICLs) when compared to the Q-LIT-OT-MS gold standard.
- QqQ-MS generated nine false-positive results due to limited mass resolution, which were effectively excluded by PLS-DA.
- Six DNA adducts/ICLs were not detected by QqQ-MS due to insufficient sensitivity, but this could be improved with selected reaction monitoring (SRM) and multiple injections.
Conclusions:
- High resolution is not strictly necessary for MS-based DNA adductomics, especially for pre-screening purposes.
- LC-QqQ-MS, when combined with statistical analysis, offers a cost-effective and comparable alternative to HRMS for DNA adductomic analysis.
- This approach broadens the accessibility of DNA adductomics for exposomics research and cancer risk assessment.
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