Direct analysis of fulvic acids adsorbed onto capped gold nanoparticles by laser desorption ionization Fourier-transform ion cyclotron resonance mass spectrometry

Γιαννόπουλος, Κωνσταντίνος; Benettoni, Pietro; Holbrook, Timothy R.; Reemtsma, Thorsten; Wagner, Stephan; Lechtenfeld, Oliver J.

doi:10.1039/d0en01253j

Cited by 10 publications

(7 citation statements)

References 45 publications

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“…Although other ionization methods may provide additional details on distinct DOM fractions, trends observed from ESI(−) measurements of solutions match well with trends observed on particle surfaces measured with laser desorption ionization. 27 For each spectrum, 256 scans were coadded in the mass range of 150−1000 m/z with 6−9 ms ion accumulation time and 4 MWord time domain (resolution at 400 m/z was ca. 500,000).…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

Legacy Effects of Sorption Determine the Formation Efficiency of Mineral-Associated Soil Organic Matter

Chen

Klotzbücher

Lechtenfeld

et al. 2022

Environ. Sci. Technol.

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Sorption of dissolved organic matter (DOM) is one major pathway in the formation of mineral-associated organic matter (MOM), but there is little information on how previous sorption events feedback to later ones by leaving their imprint on mineral surfaces and solutions ("legacy effect"). In order to conceptualize the role of legacy effects in MOM formation, we conducted sequential sorption experiments with kaolinite and gibbsite as minerals and DOM derived from forest floor materials. The MOM formation efficiency leveled off upon repeated addition of identical DOM solutions to minerals due to the retention of highly sorptive organic molecules (primarily aromatic, nitrogen-poor, hydrogen-poor, and oxygen-rich molecules), which decreased the sorption site availability and simultaneously modified the mineral surface charge. Organic− organic interactions as postulated in multilayer models played a negligible role in MOM formation. Continued exchange between DOM and MOM molecules upon repeated sorption altered the DOM composition but not the MOM formation efficiencies. Sorption-induced depletion of high-affinity compounds from solutions further decreased the MOM formation efficiencies to pristine minerals. Overall, the interplay between the differential sorptivities of DOM components and the mineral surface chemistry explains the legacy effects that contribute to the regulation of fluxes and the distribution of organic matter in the soil.

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Section: ■ Materials and Methodsmentioning

confidence: 99%

Legacy Effects of Sorption Determine the Formation Efficiency of Mineral-Associated Soil Organic Matter

Chen

Klotzbücher

Lechtenfeld

et al. 2022

Environ. Sci. Technol.

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“…thermal analysis Dufour et al, 2022;Henneron et al, 2022). LDI is known to preferentially ionize less polar, highly aromatic molecules (Blackburn et al, 2017;Solihat et al, 2019a;Giannopoulos et al, 2021). Despite these potential limitations, both our bulk and molecular-level NOSC estimates delivered the same picture: a general shift towards more reduced SOM upon FYM addition (Fig.…”

Section: Limitations Of the Approachmentioning

confidence: 54%

“…Molecular formulas were assigned based on the following rules: even electron configuration, mass range = 0 -1000 Da, mass error tolerance = +/-0.5 ppm, O/C ratio = 0 -1.2, H/C ratio = 0 -3, N/C ratio = 0 -1.5, double bond equivalents (DBE) = 0 -50; DBE-O = -10 -30; element ranges of major isotopes: 12 C = 1 -80, 13 C = 0 -1; 1 H = 1 -198, 14 N = 0 -2, 16 O = 0 -40, 32 S = 0 -1, 34 S = 0 -1). We used a larger range of H/C, DBE and DBE-O as compared to ESI spectra of aqueous WEOM extracts, because LDI is known to preferentially ionize less polar, highly aromatic fraction of WEOM (Solihat et al, 2019a;Giannopoulos et al, 2021). Isotope information ( 34 S, 13 C) was used for quality assurance but removed from the data because it represents redundant chemical information.…”

Section: Elemental Analysismentioning

confidence: 99%

Long-term effects of farmyard manure addition on soil organic matter molecular composition: C transformation as a major driver of energetic potential

Simon,

Miltner,

Mulder

et al. 2024

Preprint

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Long-term addition of farmyard manure (FYM) supports the accumulation of microbial C and soil organic matter (SOM), but the effects on energy storage remain unknown. In particular, it remains unresolved whether FYM or the stimulation of microbial transformations explains the increased microbial imprint. The latter would suggest that the accumulation of SOM transformation products controls energy storage, rather than FYM directly. We hypothesized that the overlap with original FYM signatures could be used as a measure of SOM transformation and its effect on SOM's nominal oxidation state of C (NOSC) and energetic potential ΔG0Cox. We employed solid-state laser desorption ionization Fourier transform mass spectrometry (LDI-FT-ICR-MS) to study molecular signatures of FYM samples and topsoil from four long-term field experiments receiving FYM, and unfertilized controls. In line with bulk elemental analysis, LDI-FT-ICR-MS suggested that FYM addition increased SOM's energetic potential (0.7 – 1.2 kJ/mol C). FYM addition changed SOM composition by 3 - 16% of ion abundance as compared to controls, being larger in longer-running field experiments. Markers unrelated to original FYM signatures (i.e., indirect effects) explained 67 – 84% of molecular changes while markers directly related to FYM explained only 2 – 12%. FYM addition shifted molecular composition to higher H/C, O/C and m/z, and lower aromaticity. Accumulated molecules had higher energetic potentials and were, despite being chemically similar to original FYM, elevated in mass, suggesting potential use of FYM-derived building blocks for microbial synthesis of larger molecules. Vanishing molecules showed lower energetic potential, mirroring the higher oxidation state of water-extractable organic matter, which pointed to an increased solubility of SOM. Our results indicate a uniform shift in SOM properties upon FYM addition, but highlight the role of site-specific trajectories of SOM compositional change. We discuss the implications of FYM-induced microbial transformations for energy storage and long-term stability of SOM.

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“…56 Therefore, characterization of these complex systems is a requirement for understanding the interaction of organic molecules with the particle surface and its consequences for particle fate. 56,74,75…”

Section: Reactivitymentioning

confidence: 99%

Practical considerations to optimize aquatic testing of particulate material, with focus on nanomaterials

Luederwald,

Davies,

Fernandes

et al. 2024

Environ. Sci.: Nano

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Direct analysis of fulvic acids adsorbed onto capped gold nanoparticles by laser desorption ionization Fourier-transform ion cyclotron resonance mass spectrometry

Abstract: Laser desorption ionization Fourier-transform ion cyclotron resonance mass spectrometry for direct molecular characterization of nanoparticle coronas.

Cited by 10 publications

References 45 publications

Legacy Effects of Sorption Determine the Formation Efficiency of Mineral-Associated Soil Organic Matter

Legacy Effects of Sorption Determine the Formation Efficiency of Mineral-Associated Soil Organic Matter

Long-term effects of farmyard manure addition on soil organic matter molecular composition: C transformation as a major driver of energetic potential

Practical considerations to optimize aquatic testing of particulate material, with focus on nanomaterials

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