Linking molecular composition to proton and copper binding ability of fulvic acid: A theoretical modeling approach based on FT-ICR-MS analysis

Wang, Pei; Ding, Yang; Yao, Liang; Liu, Minqin; Lin, Xiaofeng; Ye, Qianting; Shi, Zhenqing

doi:10.1016/j.gca.2021.07.019

Cited by 39 publications

(25 citation statements)

References 60 publications

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“…Solid phase extraction (SPE) was performed using Bond Elut PPL cartridges (1 g per 6 mL, Agilent) to desalinate and concentrate the DOM solutions according to methods established in previous studies. , The details of the SPE process are presented in SI. Using this method, the extraction efficiency of DOM was above 62% based on DOC recovery, which was close to the recovery efficiency reported previously. ,, In addition, any H 2 C 2 O 4 left in the experiments that was used for dissolving birnessite was also removed during the SPE process, which did not affect the FT-ICR-MS analysis.…”

Section: Materials and Methodsmentioning

confidence: 99%

“…Using this method, the extraction efficiency of DOM was above 62% based on DOC recovery, which was close to the recovery efficiency reported previously. 28,35,46 In addition, any H 2 C 2 O 4 left in the experiments that was used for dissolving birnessite was also removed during the SPE process, which did not affect the FT-ICR-MS analysis.…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

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Coupled Sorption and Oxidation of Soil Dissolved Organic Matter on Manganese Oxides: Nano/Sub-nanoscale Distribution and Molecular Transformation

Ding

Liu

et al. 2022

Environ. Sci. Technol.

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In soil environments, the sequestration and transformation of organic carbon are closely associated with soil minerals. Birnessite (MnO2) is known to strongly interact with soil dissolved organic matter (DOM), but the microscopic distribution and molecular transformation of soil DOM on birnessite are still poorly understood. In this study, the coupled sorption and oxidation of soil DOM on birnessite were investigated at both the microscopic scale and the molecular level. Spherical aberration corrected scanning transmission electron microscopy (Cs-STEM) results revealed, at the nano- to sub-nanoscale, that DOM was located both on the surfaces and within the interflakes or pore spaces of birnessite, and DOM within the interflakes displayed a higher oxidation state than that on the surfaces. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) results suggested that a portion of phenolic compounds were preferentially sorbed and oxidized, resulting in the formation of compounds with higher oxygen contents and polymeric products. Our Cs-STEM and FT-ICR-MS results highlighted the significance of organo-mineral associations in the microscopic mineral structure for the reactivity of organic carbon and provided the molecular evidence for the transformation of soil DOM by birnessite, which contributed to the understanding of the dynamics of soil dissolved organic carbon.

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Section: Materials and Methodsmentioning

confidence: 99%

Section: ■ Materials and Methodsmentioning

confidence: 99%

Coupled Sorption and Oxidation of Soil Dissolved Organic Matter on Manganese Oxides: Nano/Sub-nanoscale Distribution and Molecular Transformation

Ding

Liu

et al. 2022

Environ. Sci. Technol.

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“…To identify the representative molecular groups of soil DOM, associations between n A from WHAM 7 calculations and the relative intensities of DOM molecules from FT-ICR-MS analysis were quantified using the Spearman correlation analysis. The common molecules presented in at least four DOM samples were used for correlation analysis according to previous studies, ,, in which the relative intensities of the common molecules in 24 soil DOM were tabulated together for correlation analysis with n A values. Therefore, molecules presented in less than four soil DOM were not considered in correlation analysis, but these molecules only accounted for, on average, about 4% of all molecules in each soil DOM based on the intensities of molecules.…”

Section: Methodsmentioning

confidence: 99%

“…The molecular model, Vienna Soil-Organic-Matter Modeler (VSOMM), is a promising tool to describe the chemical compositions and structures of organic matter. − Our recent work on theoretical modeling of the Suwannee river fulvic acid (FA) based on FT-ICR-MS data and VSOMM revealed that the heterogeneous FA molecules can be identified to three representative groups of molecules, which provided a new view on the simplification of the heterogeneity of FA molecules based on the molecular data and the molecular mixture model . However, the chemical compositions of soil DOM across strong environmental gradients were reported to be extreme complex and may be much more diverse than those observed in aquatic systems, ,, which have not yet been revealed and understood at the molecular level.…”

Section: Introductionmentioning

confidence: 99%

“…However, the chemical compositions of soil DOM across strong environmental gradients were reported to be extreme complex and may be much more diverse than those observed in aquatic systems, ,, which have not yet been revealed and understood at the molecular level. Developing theoretical models for soil DOM should specifically account for both the heterogeneity and chemodiversity of soil DOM molecules, which, in principle, can be accommodated by the molecular mixture modeling approach developed in our previous studies on model humic substances. , If successful, this type of modeling approach is of environmental significance for quantifying the proton and metal binding ability of soil DOM from different sources in natural environments.…”

Section: Introductionmentioning

confidence: 99%

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Unified Modeling Approach for Quantifying the Proton and Metal Binding Ability of Soil Dissolved Organic Matter

Ding

et al. 2022

Environ. Sci. Technol.

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Soil dissolved organic matter (DOM) is composed of a mass of complex organic compounds in soil solutions and significantly affects a range of (bio)geochemical processes in soil environment. However, how the chemical complexity (i.e., heterogeneity and chemodiversity) of soil DOM molecules affects their proton and metal binding ability remains unclear, which limits our ability for predicting the environmental behavior of DOM and metals. In this study, we developed a unified modeling approach for quantifying the proton and metal binding ability of soil DOM based on Cu titration experiments, Fourier transform ion cyclotron resonance mass spectrometry data, and molecular modeling method. Although soil DOM samples from different regions have enormously heterogeneous and diverse properties, we found that the molecules of soil DOM can be divided into three representative groups according to their Cu binding capacity. Based on the molecular models for individual molecular groups and the relative contributions of each group in each soil DOM, we were able to further develop molecular models for all soil DOM to predict their molecular properties and proton and metal binding ability. Our results will help to develop mechanistic models for predicting the reactivity of soil DOM from various sources.

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Towards a better understanding of the role of Fe cycling in soil for carbon stabilization and degradation

et al. 2022

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Iron (Fe) minerals play an important role in stabilizing soil organic carbon (SOC). Fe-mediated SOC protection is mainly achieved through adsorption, co-precipitation, or aggregation. However, newly emerging evidence indicates that the electron transfer role of Fe exerts a crucial influence upon SOC turnover. In this review, we address the pathways of Fe mineral-associated soil organic carbon (Fe-SOC) formation and decomposition, and summarize the Fe-mediated biogeochemical, including redox reactions, and physical processes that control SOC cycling. The reduction of Fe can release SOC from Fe-SOC coprecipitates and Fe(III) cemented micro-aggregates, with the process also releasing CO2 from the metabolic coupling of SOC oxidation and Fe reduction. The abiotic oxidation of Fe(II) by oxidants can also oxidize SOC to produce CO2 due to reactive oxygen species production. Therefore, the functional roles of Fe on SOC sequestration may be a double-edged sword, and these processes are rarely explored concurrently. We conclude that the roles of Fe minerals in SOC stability depend on the properties of the Fe mineral, edaphic properties, and anthropogenic influence. We highlight knowledge gaps and promising directions of future research in redox-dynamic environments to optimize carbon storage in soil. Graphical Abstract

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Linking molecular composition to proton and copper binding ability of fulvic acid: A theoretical modeling approach based on FT-ICR-MS analysis

Cited by 39 publications

References 60 publications

Coupled Sorption and Oxidation of Soil Dissolved Organic Matter on Manganese Oxides: Nano/Sub-nanoscale Distribution and Molecular Transformation

Coupled Sorption and Oxidation of Soil Dissolved Organic Matter on Manganese Oxides: Nano/Sub-nanoscale Distribution and Molecular Transformation

Unified Modeling Approach for Quantifying the Proton and Metal Binding Ability of Soil Dissolved Organic Matter

Towards a better understanding of the role of Fe cycling in soil for carbon stabilization and degradation

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