Improved Dynamic Range, Resolving Power, and Sensitivity Achievable with FT-ICR Mass Spectrometry at 21 T Reveals the Hidden Complexity of Natural Organic Matter DOI
William Bahureksa, Thomas Borch, Robert B. Young

et al.

Analytical Chemistry, Journal Year: 2022, Volume and Issue: 94(32), P. 11382 - 11389

Published: Aug. 2, 2022

Fourier transform ion-cyclotron resonance mass spectrometry (FT-ICR MS) is the only analyzer that can resolve molecular complexity of natural organic matter at level elemental composition assignment. Here, we leverage high dynamic range, resolving power, resistance to peak coalescence, and maximum ion number trapping duration in a custom built, 21 tesla hybrid linear trap /FT-ICR spectrometer for dissolved standard (Suwanne River Fulvic Acid). We compare effect peak-picking threshold (3σ, 4σ, 5σ, 6σ) on assignments, measurement accuracy, range 6.3 s transient across m/z 200-1200 comprises highest achieved power broadband FT-ICR spectrum collected date. More than 36 000 species are assigned with signal magnitude greater 3σ root-mean-square error ppb, most identified reported date matter. identify 18O 17O isotopologues isobaric overlaps order few electrons wide (up 1000) leveraging powers (3 200) achievable by T MS increased ∼30% through absorption mode data processing. Elemental compositions unique span compositional aromaticity not detected higher thresholds. Furthermore, provide catalogue widely utilized reference (SRFA) analytical community performing complex mixture analysis This instrument available free charge scientists worldwide.

Language: Английский

Deciphering dissolved organic matter by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS): from bulk to fractions and individuals DOI Creative Commons
Yulin Qi, Qiaorong Xie, Junjian Wang

et al.

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

Citations

113

Advances in gas sensors and electronic nose technologies for agricultural cycle applications DOI
Thara Seesaard, Neeraj Goel, Mahesh Kumar

et al.

Computers and Electronics in Agriculture, Journal Year: 2022, Volume and Issue: 193, P. 106673 - 106673

Published: Jan. 10, 2022

Language: Английский

Citations

103

Direct and Indirect Electron Transfer Routes of Chromium(VI) Reduction with Different Crystalline Ferric Oxyhydroxides in the Presence of Pyrogenic Carbon DOI
Zibo Xu,

Yulu Yu,

Xiaoyun Xu

et al.

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(3), P. 1724 - 1735

Published: Jan. 3, 2022

Electron transfer mediated by iron minerals is considered as a critical redox step for the dynamics of pollutants in soil. Herein, we explored reduction process Cr(VI) with different crystalline ferric oxyhydroxides presence pyrogenic carbon (biochar). Both low- and high-crystallinity induced immobilization mainly via sorption process, limited process. However, was inspired copresence biochar. Low-crystallinity oxyhydroxide had an intense chemical combination biochar strong inner-sphere complexation, leading to indirect electron route reduction, that is, first transferred from mineral through C–O–Fe binding then Fe(III)/Fe(II) transformation on oxyhydroxides. With increasing crystallinity oxyhydroxides, direct between became main avenue reduction. The suppressed due less Cr(VI), biochar, higher stability. This study demonstrates mechanisms involving change crystallization which would affect geochemical contaminants carbon.

Language: Английский

Citations

73

Chemical composition, sources, and ecological effect of organic phosphorus in water ecosystems: a review DOI Creative Commons
Weiying Feng,

Tengke Wang,

Yuanrong Zhu

et al.

Carbon Research, Journal Year: 2023, Volume and Issue: 2(1)

Published: March 15, 2023

Abstract Phosphorus (P) affects the water–air CO 2 flux through primary productivity, and changes of carbon cycle ecological environment in global world. Organic phosphorus (Po) is an important P component water environments. Various processes control formation transformation Po outbreaks algal blooms. Here, research topics on over past 50 years are systematically reviewed to understand progress (i) pretreatment techniques various media, (ii) technical methods qualitative quantitative chemical composition bioavailability, (iii) source analysis factors affecting different media environments biogeochemical processes, (iv) interactions among Po, organic matter, minerals, their environmental behaviors, (v) quantification material exchanges at sediment–water interface, interfacial effects. Finally, future directives regarding discussed. The findings provided scientific basis formulate revise standards for nutrients a better understanding eutrophication its control. Graphical

Language: Английский

Citations

69

Soil metabolomics - current challenges and future perspectives DOI Creative Commons
Robert W. Brown, Michaela Reay, Florian Centler

et al.

Soil Biology and Biochemistry, Journal Year: 2024, Volume and Issue: 193, P. 109382 - 109382

Published: March 12, 2024

Soil is an extremely complex and dynamic matrix, in part, due to the wide diversity of organisms living within it. organic matter (SOM) fundamental substrate on which delivery ecosystem services depends, providing metabolic fuel drive soil function. As such, studying metabolome (the concentration low molecular weight metabolites), as a subset SOM, holds potential greatly expand our understanding behaviour, fate, interaction functional significance small molecules soil. Encompassing range chemical classes (including amino acids, peptides, lipids carbohydrates) large number individual (ca. n = 105 106), resultant (indirect) output several layers biological hierarchy, namely metagenome, metatranscriptome metaproteome. it may also provide support validation for these "multi-omics" datasets. We present case increased use untargeted metabolomics biochemistry, particularly furthering functions driving SOM composition biogeochemical cycling. Further, we discuss scale challenge terms metabolite extraction, analysis interpretation plant-soil-microbial systems. Lastly, highlight key knowledge gaps currently limit metabolomic approaches better understand processes, including: (i) datasets; (ii) source, emission fate soil-derived volatile compounds (VOCs), (iii) assessing temporal fluxes metabolites, (iv) monitoring ecological interactions rhizosphere. While application science still its relative infancy, importance biochemical system relation regulation, management underpinning further elucidating links between organisms, well ability community process cycle nutrients.

Language: Английский

Citations

24

Spatial patterns and environmental functions of dissolved organic matter in grassland soils of China DOI Creative Commons
Peng Zhou, Long Tian,

Nigel Graham

et al.

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

Published: July 28, 2024

Soil dissolved organic matter (DOM) is crucial to atmospheric, terrestrial and aquatic environments as well human life. Here, by characterizing DOM from 89 grassland soils throughout China, we reveal the spatial association between geochemistry in dry season vs annual ecosystem exchange cancer cases. The humic-like high molecular weight (3.4–25 kDa) fractions with lower biodegradability, decline northern southern regions of are correlated soil respiration net productivity at continental scale. <1.2 kDa proteinaceous could serve a geographical indicator nasopharyngeal incidence mortality, while 3.4–25 humified potentially associated pancreatic cases (P < 0.05). Our findings highlight that exploiting environmental functions mitigating negative impacts necessary, require actions tailored local conditions. critical processes humans. Here authors variations different playing varied roles carbon health.

Language: Английский

Citations

22

Long-term effects of manure addition on soil organic matter molecular composition: Carbon transformation as a major driver of energetic potential DOI Creative Commons
Carsten Simon, Anja Miltner, Ines Mulder

et al.

Soil Biology and Biochemistry, Journal Year: 2025, Volume and Issue: unknown, P. 109755 - 109755

Published: Feb. 1, 2025

Language: Английский

Citations

3

PFAS Analysis with Ultrahigh Resolution 21T FT-ICR MS: Suspect and Nontargeted Screening with Unrivaled Mass Resolving Power and Accuracy DOI
Robert B. Young, Nasim E. Pica, Hamidreza Sharifan

et al.

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(4), P. 2455 - 2465

Published: Jan. 31, 2022

Per- and polyfluoroalkyl substances (PFASs) are a large family of thousands chemicals, many which have been identified using nontargeted time-of-flight Orbitrap mass spectrometry methods. Comprehensive characterization complex PFAS mixtures is critical to assess their environmental transport, transformation, exposure, uptake. Because 21 tesla (T) Fourier-transform ion cyclotron resonance (FT-ICR MS) offers the highest available resolving power sub-ppm errors across wide molecular weight range, we developed T FT-ICR MS method screen for PFASs in an aqueous film-forming foam (AFFF) suspect screening, targeted formula database (C, H, Cl, F, N, O, P, S; ≤865 Da), isotopologues, Kendrick-analogous difference networks (KAMDNs). False-positive identifications natural organic matter (NOM) sample, served as negative control, suggested that minimum length 3 should be imposed when annotating CF2-homologous series with positive defects. We putatively 163 known during well 134 novel including suspected polyethoxylated perfluoroalkane sulfonamide series. This study shows analysis can provide unique insights into composition expand our understanding chemistries impacted matrices.

Language: Английский

Citations

64

Data-Based Chemical Class Regions for Van Krevelen Diagrams DOI
Juliana R. Laszakovits, Allison A. MacKay

Journal of the American Society for Mass Spectrometry, Journal Year: 2021, Volume and Issue: 33(1), P. 198 - 202

Published: Dec. 7, 2021

Ultrahigh resolution mass spectrometry (UHR-MS) is commonly used to characterize natural organic matter (NOM). The complexity of both NOM and the data set produced make visualization challenging. Van Krevelen diagrams─plots component hydrogen/carbon (H/C) against oxygen/carbon (O/C) elemental ratios─have become a popular way visualize chemical formulas identified by UHR-MS. Different regions on van diagram have been attributed different classes; however, classifications vary between studies lack standard definitions. Here, were obtained from public databases create H/C O/C ranges for amino sugar, carbohydrate, lignin, lipid, peptide, tannin classes diagrams. recommended are presented in table can be adapted any analysis software programs. here agreed reasonably well with previous literature peptide regions. However, region appears at lower ratio values wider range compared studies. herein strongly use as consistent reference points future characterization aid discussion readily compare

Language: Английский

Citations

63

Nitrogen Enrichment during Soil Organic Matter Burning and Molecular Evidence of Maillard Reactions DOI
William Bahureksa, Robert B. Young, Amy M. McKenna

et al.

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(7), P. 4597 - 4609

Published: March 9, 2022

Wildfires in forested watersheds dramatically alter stored and labile soil organic matter (SOM) pools the export of dissolved (DOM). Ecosystem recovery after wildfires depends on microbial communities revegetation therefore is limited by availability nutrients, such as nitrogen-containing labile, water-soluble compounds. However, SOM byproducts produced at different wildfire intensities are poorly understood, leading to difficulties assessing severity predicting ecosystem recovery. In this work, water-extractable (WEOM) from laboratory microcosms burned discrete temperatures was characterized ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry study impacts fire temperature DOM composition. The molecular composition derived burn indicated that were enriched with heating composed a wide range aromatic features oxidation states. Mass difference-based analysis also suggested products formed during could be modeled using transformations along Maillard reaction pathway. enrichment N-containing burning has important implications for downstream water quality.

Language: Английский

Citations

48