Soil Organic Matter Characterization by Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR MS): A Critical Review of Sample Preparation, Analysis, and Data Interpretation

Environmental Science & Technology, Journal Year: 2021, Volume and Issue: 55(14), P. 9637 - 9656

Published: July 7, 2021

The biogeochemical cycling of soil organic matter (SOM) plays a central role in regulating health, water quality, carbon storage, and greenhouse gas emissions. Thus, many studies have been conducted to reveal how anthropogenic climate variables affect sequestration nutrient cycling. Among the analytical techniques used better understand speciation transformation SOM, Fourier transform ion cyclotron resonance mass spectrometry (FTICR MS) is only technique that has sufficient resolving power separate accurately assign elemental compositions individual SOM molecules. global increase application FTICR MS address complexity highlighted challenges opportunities associated with sample preparation, analysis, spectral interpretation. Here, we provide critical review recent strategies for characterization by emphasis on collection, data Data processing visualization methods are presented suggested workflows detail considerations needed molecular information derived from MS. Finally, highlight current research gaps, biases, future directions improve our understanding chemistry within terrestrial ecosystems.

Language: Английский

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Deciphering dissolved organic matter by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS): from bulk to fractions and individuals

Carbon Research, Journal Year: 2022, Volume and Issue: 1(1)

Published: June 18, 2022

Abstract Exploring the source, transformation pathways, and fate of natural organic matter (NOM) is critical to understanding regional/global carbon cycle budget. The dissolved fraction NOM, i.e., (DOM), a complex mixture resulting from plant, animal microbial plays crucial role in many biogeochemical processes at land-ocean-atmosphere interfaces. advance Fourier transform ion cyclotron resonance mass spectrometer (FT-ICR MS) makes detailed characterization DOM molecular level possible. On other hand, elucidation sample also presents significant analytical challenges, these challenges act as driving force for instrumentation methodology development on FT-ICR MS. This review article has been written aid those working biogeochemistry, environmental atmospheric chemistry, related areas which investigate elemental cycles transformations. First, fundamental theory, historical perspective, recent advances field have introduced. geological samples continues present it become experimental methods. These achievements analysis had an impact upon fields science, geochemistry, chemistry. Next, varieties applications MS described, followed by our view future this technique earth science research. We believe that covers essential pairing collectively offers geochemical scientists substantial resource their Graphical abstract

Language: Английский

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Dissolved Organic Matter Photoreactivity Is Determined by Its Optical Properties, Redox Activity, and Molecular Composition

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(16), P. 6703 - 6711

Published: April 11, 2023

Predicting the formation of photochemically produced reactive intermediates (PPRI) during irradiation dissolved organic matter (DOM) has remained challenging given complex nature this material and differences in PPRI mechanisms. We investigate role DOM composition photoreactivity using 48 samples that span range freshwater systems wastewater. relate quantum yields for excited triplet-state (fTMP), singlet oxygen (Φ1O2), hydroxylating species (Φ•OH) to determined spectroscopy, Fourier-transform ion cyclotron resonance mass spectrometry, electron-donating capacity (EDC). fTMP Φ1O2 follow similar trends are correlated with bulk properties derived from UV–vis spectra EDC. In contrast, no individual property can be used predict Φ•OH. At molecular level, subset is positively both Φ•OH EDC distinct formulas related Φ1O2, demonstrating •OH 1O2 formed different fractions. Multiple linear regressions each parameters multiple techniques, complementary methods ideal characterizing because technique only a DOM.

Language: Английский

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Direct Analysis of Marine Dissolved Organic Matter Using LC-FT-ICR MS

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(10), P. 4637 - 4647

Published: March 1, 2024

Marine dissolved organic matter (DOM) is an important component of the global carbon cycle, yet its intricate composition and sea salt matrix pose major challenges for chemical analysis. We introduce a direct injection, reversed-phase liquid chromatography ultrahigh resolution mass spectrometry approach to analyze marine DOM without need solid-phase extraction. Effective separation achieved with large chromatographic column extended isocratic aqueous step. Postcolumn dilution sample flow buffer-free solvents implementing counter gradient reduced buildup in ion source resulted excellent repeatability. With this method, over 5,500 unique molecular formulas were detected from just 5.5 nmol 100 μL filtered Arctic Ocean seawater. observed highly linear detector response variable concentrations high robustness against matrix. Compared extracted DOM, our injection method demonstrated superior sensitivity heteroatom-containing DOM. The analysis seawater offers fast simple preparation avoids fractionation introduced by facilitates studies environments, where only minimal volume available e.g. sediment pore water, ice cores, or permafrost soil solution. small requirement also supports higher spatial (e.g., soils) temporal culture experiments). Chromatographic adds further information formulas, enhancing understanding biogeochemistry, chemodiversity, ecological processes.

Language: Английский

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Thermal responses of dissolved organic matter under global change

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Jan. 17, 2024

The diversity of intrinsic traits different organic matter molecules makes it challenging to predict how they, and therefore the global carbon cycle, will respond climate change. Here we develop an indicator compositional-level environmental response for dissolved quantify aggregated individual that positively negatively associate with warming. We apply assess thermal sediment in 480 aquatic microcosms along nutrient gradients on three Eurasian mountainsides. Organic consistently temperature change within across contrasting zones. At a compositional level, warmer sites has stronger shows functional reorganization towards lower thermodynamic favorability microbial decomposition. is more sensitive warming at higher nutrients, increased sensitivity up 22% each additional 1 mg L

Language: Английский

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Exploring the fate of dissolved organic matter at the molecular level in the reactive electrochemical ceramic membrane system using fluorescence spectroscopy and FT-ICR MS

Water Research, Journal Year: 2021, Volume and Issue: 210, P. 117979 - 117979

Published: Dec. 19, 2021

Language: Английский

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Application of Fourier transform ion cyclotron resonance mass spectrometry in molecular characterization of dissolved organic matter

Science China Earth Sciences, Journal Year: 2022, Volume and Issue: 65(12), P. 2219 - 2236

Published: Sept. 28, 2022

Language: Английский

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Molecular composition of dissolved organic matter across diverse ecosystems: Preliminary implications for biogeochemical cycling

Journal of Environmental Management, Journal Year: 2023, Volume and Issue: 344, P. 118559 - 118559

Published: July 5, 2023

Language: Английский

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Probing Molecular-Level Dynamic Interactions of Dissolved Organic Matter with Iron Oxyhydroxide via a Coupled Microfluidic Reactor and an Online High-Resolution Mass Spectrometry System

Environmental Science & Technology, Journal Year: 2023, Volume and Issue: 57(7), P. 2981 - 2991

Published: Feb. 7, 2023

The interactions between dissolved organic matter (DOM) and iron (Fe) oxyhydroxide are crucial in regulating the biogeochemical cycling of nutrients elements, including preservation carbon soils. mechanisms DOM molecular assembly on mineral surfaces have been extensively studied at mesoscale with equilibrium experiments, yet molecular-level evolution DOM-mineral interface under dynamic interaction conditions is not fully understood. Here, we designed a microfluidic reactor coupled an online solid phase extraction (SPE)-LC-QTOF MS system to continually monitor changes composition during flowing contact Fe circumneutral pH, which simulates soil minerals interacting constant input. Time-series UV-visible absorption spectra mass spectrometry data showed that after aromatic moieties were first preferentially sequestered by pristine surface, adsorption nonaromatic molecules greater hydrophobicity, lower acidity, weights (<400) from new solutions was favored. This accompanied transition surface chemistry-dominated organic-organic interaction-dominated adsorption. These findings provide direct evidence zonal model taking dynamics interfacial into consideration. study also shows microfluidics high-resolution (HRMS) promising experimental platform for probing microscale environmental integrating situ reactions, sample pretreatment, automatic analysis.

Language: Английский

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Will various interpretation strategies of the same ultrahigh‐resolution mass spectrometry data tell different biogeochemical stories? A first assessment based on natural aquatic dissolved organic matter

Limnology and Oceanography Methods, Journal Year: 2023, Volume and Issue: 21(6), P. 320 - 333

Published: May 10, 2023

Abstract Fourier ion cyclotron resonance mass spectrometry (FT‐ICR MS), one of the state‐of‐the‐art ultrahigh‐resolution techniques, is widely used in dissolved organic matter (DOM) research. As research that focuses on identifying DOM molecular fingerprints increases tremendously, there and will be an urgent need to compare among studies. Different groups usually use various types data processing interpretation strategies. It critical explore if different strategies impact comparability FT‐ICR MS results their biogeochemical interpretations. To address this question, we selected samples along a freshwater‐to‐marine continuum measured by negative‐ion mode electrospray ionization MS. We interpreted raw using strategies, compared evaluated strategy‐induced effects Our show total 3827 formulas account for 91.6% ± 4.1% (on average) intensity are assigned all while 6521 8.4% not commonly three conclude (i) do significantly affect geochemical stories relied composition, (ii) comparison based gives more reliable than formular number alone. Moreover, also provide (by our strategies) community interpretation. aim call attention improving facilitating integration composition global

Language: Английский

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