Linking the molecular composition of autochthonous dissolved organic matter to source identification for freshwater lake ecosystems by combination of optical spectroscopy and FT-ICR-MS analysis

Li, Shasha; He, Zhongqi; Tang, Zhi; Liu, Leizhen; Hou, Junwen; Li, Tingting; Zhang, Yahe; Shi, Quan; Giesy, John P.; Wu, Fengchang

doi:10.1016/j.scitotenv.2019.134764

Cited by 117 publications

(39 citation statements)

References 61 publications

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“…S2). Differences in molecular composition between seawater and sea ice are in agreement with the previous observations in sea ice DOM (Longnecker, 2015;Retelletti Brogi et al, 2018) and lake ice DOM (Liu et al, 2020;Santibáñez et al, 2019;Xu et al, 2020). implying a selective transport of DOM with less complex, aliphatic compounds -rather than larger aromatic oligomers, during ice formation.…”

Section: Sea Icesupporting

confidence: 90%

Compositions of dissolved organic matter in the ice-covered waters above the Aurora hydrothermal vent system, Gakkel Ridge, Arctic Ocean

Sert

Niemann

Reeves

et al. 2022

Preprint

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Abstract. Hydrothermal vents modify and displace subsurface dissolved organic matter (DOM) into the ocean. Once in the ocean, this DOM is transported together with elements, particles, dissolved gases, and biomass along with the neutrally buoyant plume layer. Considering the number and extent of actively venting hydrothermal sites in the oceans, their contribution to the oceanic DOM pool may be substantial. Here, we investigate the dynamics of DOM in relation to hydrothermal venting and related processes at the as-yet unexplored Aurora hydrothermal vent field within the ultraslow spreading Gakkel Ridge in the Arctic Ocean at 82.9° N. We examined the vertical distribution of DOM composition from sea ice to deep waters at six hydrocast stations distal to the active vent and its neutrally buoyant plume layer. In comparison to background seawater, we found that the DOM in waters directly affected by the hydrothermal plume was composed of lower numbers of molecular formulas and 5–10 % less abundant compositions associated with the molecular categories related to lipid and protein-like compounds. Samples that were not directly affected by the plume, on the other hand, were chemically more diverse and had a higher percentage of chemical formulas associated with the carbohydrate-like category. We suggest, therefore, that hydrothermal processes at Aurora may influence the DOM distribution in the bathypelagic ocean by spreading more thermally and/or chemically induced compositions, while DOM compositions in epipelagic and mesopelagic layers are mainly governed by the microbial carbon pump dynamics, and sea ice surface water interactions.

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Section: Sea Icesupporting

confidence: 90%

Compositions of dissolved organic matter in the ice-covered waters above the Aurora hydrothermal vent system, Gakkel Ridge, Arctic Ocean

Sert

Niemann

Reeves

et al. 2022

Preprint

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“…The double bond equivalence (DBE) and AI mod were calculated to indicate the dynamic changes in aromaticity and oxidation state of DOM; for example, a lower value of AI mod was found in labile and semilabile fractions than that of refractory molecules, indicating the negative relationship between aromaticity and bioavailability of DOM . The molecular lability (MLB L ) was used to estimate the lability of DOM, and a higher MLB L meant DOM with a higher lability . Aliquots of filtered water were acidified with trace metal grade HNO 3 and then analyzed for the changes in dissolved Fe levels between the “Control” groups and “Algae” treatments (indicating iron reduction , ) by ICP–MS .…”

Section: Methodsmentioning

confidence: 99%

“…Algal organic matter (AOM) has been reported to play a critical role in controlling microbial Hg methylation ( e.g. , by fueling the metabolism of microbial methylators). , The global occurrences of algal blooms have expanded during past decades, , and some dominating cyanobacteria release high amounts of AOM, a major fraction of dissolved organic matter (DOM), into water, especially in shallow lakes. , However, the complexity of AOM compositions and its dynamic changes in eutrophic shallow lakes make it difficult to understand microbial Hg methylation in water. For example, during algal decomposition, AOM was depleted in highly unsaturated, high-oxygen molecules and enriched in aliphatic, highly unsaturated, low-oxygen molecules, and these dynamic changes in AOM compositions in turn impacted microbial diversity and could possibly regulate microbial Hg methylation in water.…”

Section: Introductionmentioning

confidence: 99%

Algal Organic Matter Drives Methanogen-Mediated Methylmercury Production in Water from Eutrophic Shallow Lakes

Lei

Zhang

Zhu

et al. 2021

Environ. Sci. Technol.

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Algal blooms bring massive amounts of algal organic matter (AOM) into eutrophic lakes, which influences microbial methylmercury (MeHg) production. However, because of the complexity of AOM and its dynamic changes during algal decomposition, the relationship between AOM and microbial Hg methylators remains poorly understood, which hinders predicting MeHg production and its bioaccumulation in eutrophic shallow lakes. To address that, we explored the impacts of AOM on microbial Hg methylators and MeHg production by characterizing dissolved organic matter with Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) and three-dimensional excitation-emission matrix (3D-EEM) fluorescence spectroscopy and quantifying the microbial Hg methylation gene hgcA. We first reveal that the predominance of methanogens, facilitated by eutrophication-induced carbon input, could drive MeHg production in lake water. Specifically, bioavailable components of AOM (i.e., CHONs such as aromatic proteins and soluble microbial byproduct-like materials) increased the abundances (Archaea-hgcA gene: 438–2240% higher) and activities (net CH4 production: 16.0–44.4% higher) of Archaea (e.g., methanogens). These in turn led to enhanced dissolved MeHg levels (24.3–15,918% higher) for three major eutrophic shallow lakes in China. Nevertheless, our model results indicate that AOM-facilitated MeHg production could be offset by AOM-induced MeHg biodilution under eutrophication. Our study would help reduce uncertainties in predicting MeHg production, providing a basis for mitigating the MeHg risk in eutrophic lakes.

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“…to their heteroatoms-richer nature than NOM 5,48,56 . On the other hand, microbial extracellular polymeric substances and cell lysis-derived organic compounds are important biological X-DBPs precursors abundant in WWTPs during disinfection process 57 .…”

Section: Content Si5 Environmental Implicationmentioning

confidence: 99%

Development and Application of a High-Precision Algorithm for Nontarget Identification of Organohalogens Based on Ultrahigh-Resolution Mass Spectrometry

Fujii

Kwon

2020

Anal. Chem.

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The brominated and/or chlorinated organic compounds (referred to as organohalogens) are frequently detected in natural and engineered environments. However, the ultrahigh resolution mass spectrometry (UHR-MS)-based non-target identification of the organohalogens remains challenging due to the presence of vast number of halogenated and non-halogenated organic molecules in the same aqueous sample. In this study, a new algorithm, namely NOMDBP Code, was developed, based on natural organic matter (NOM) chemistry, to simultaneously identify organohalogens and non-organohalogens from the UHR-MS spectra of natural and engineered waters. In addition to isotopic pattern extraction, for the first time, three optional filter rules (namely selection of minimum non oxygen heteroatoms, inspection of newly formed halogenated disinfection byproducts [X23 DBPs] and precursors) were incorporated in our code, which can accurately identify DBPs associated peaks and further elucidate the X-DBPs generation and transformation mechanisms. The formulae assignment rate against previously reported 2,815 unique organohalogens and their 11,583 isotopologues was determined to be >97%. Application of our algorithm to disinfected NOM indicated that oxygen-containing X-DBPs species accounted for a majority of X-DBPs. Further, brominated X-DBPs (Br-DBPs) during disinfection process were characterized by higher degree of unsaturation compared to chlorinated X-DBPs (Cl-DBPs). Our algorithm also suggested that, in addition to electrophilic substitution and electrophilic addition reactions, the decomposition/transformation is another important mechanism in Br-DBPs formation. Results of this study highlight the superior potential of this code to efficiently detect yet-unknown organohalogens (including organohalogens with non-oxygen heteroatoms) in a non-target manner and identify their generation mechanism during the disinfection process File list (3) download file view on ChemRxiv DBP paper.pdf (1.10 MiB) download file view on ChemRxiv DBP paper_SI.pdf (2.69 MiB) download file view on ChemRxiv Supporting Information SI1 DBP list.xls (523.00 KiB)

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Linking the molecular composition of autochthonous dissolved organic matter to source identification for freshwater lake ecosystems by combination of optical spectroscopy and FT-ICR-MS analysis

Cited by 117 publications

References 61 publications

Compositions of dissolved organic matter in the ice-covered waters above the Aurora hydrothermal vent system, Gakkel Ridge, Arctic Ocean

Compositions of dissolved organic matter in the ice-covered waters above the Aurora hydrothermal vent system, Gakkel Ridge, Arctic Ocean

Algal Organic Matter Drives Methanogen-Mediated Methylmercury Production in Water from Eutrophic Shallow Lakes

Development and Application of a High-Precision Algorithm for Nontarget Identification of Organohalogens Based on Ultrahigh-Resolution Mass Spectrometry

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