Reviews and syntheses: Opportunities for robust use of peak intensities from high-resolution mass spectrometry in organic matter studies

Kew, William R.; Myers-Pigg, Allison N.; Chang, Christine H.; Colby, Sean M.; Eder, Josie G.; Tfaily, Malak M.; Hawkes, Jeffrey; Chu, Rosalie K.; Stegen, James C.

doi:10.5194/bg-21-4665-2024

Title: Reviews and syntheses: Opportunities for robust use of peak intensities from high-resolution mass spectrometry in organic matter studies

Journal Article · 28 October 2024 · Biogeosciences (Online)

DOI: https://doi.org/10.5194/bg-21-4665-2024 · OSTI ID:2475440

^[1];

^[2]; Chang, Christine H. ^[2]; Colby, Sean M. ^[2]; Eder, Josie G. ^[1]; Tfaily, Malak M. ^[3]; Hawkes, Jeffrey ^[4]; Chu, Rosalie K. ^[1];

^[5]

Environmental Molecular Sciences Laboratory, Richland, WA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
University of Arizona, Tucson, AZ (United States)
University of Uppsala (Sweden)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Washington State University, Pullman, WA (United States)

Earth's biogeochemical cycles are intimately tied to the biotic and abiotic processing of organic matter (OM). Spatial and temporal variations in OM chemistry are often studied using direct infusion, high-resolution Fourier transform mass spectrometry (FTMS). An increasingly common approach is to use ecological metrics (e.g., within-sample diversity) to summarize high-dimensional FTMS data, notably Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). However, problems can arise when FTMS peak-intensity data are used in a way that is analogous to abundances in ecological analyses (e.g., species abundance distributions). Using peak-intensity data in this way requires the assumption that intensities act as direct proxies for concentrations. Here, we show that comparisons of the same peak across samples (within-peak) may carry information regarding variations in relative concentration, but comparing different peaks (between-peak) within or between samples does not. We further developed a simulation model to study the quantitative implications of using peak intensities to compute ecological metrics (e.g., intensity-weighted mean properties and diversity) that rely on information about both within-peak and between-peak shifts in relative abundance. We found that, despite analytical limitations in linking concentration to intensity, ecological metrics often perform well in terms of providing robust qualitative inferences and sometimes quantitatively accurate estimates of diversity and mean molecular characteristics. We conclude with recommendations for the robust use of peak intensities for natural organic matter studies. A primary recommendation is the use and extension of the simulation model to provide objective guidance on the degree to which conceptual and quantitative inferences can be made for a given analysis of a given dataset. Broad use of this approach can help ensure rigorous scientific outcomes from the use of FTMS peak intensities in environmental applications.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: Environmental Molecular Sciences Laboratory; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2475440

Report Number(s):: PNNL-SA--179733

Journal Information:: Biogeosciences (Online), Journal Name: Biogeosciences (Online) Journal Issue: 20 Vol. 21; ISSN 1726-4189

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: United States

Language:: English

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