Fenton-Chemistry-Based Oxidative Modification of Proteins Reflects Their Conformation

Nehls, Thomas; Heymann, Tim; Meyners, Christian; Hausch, Felix; Lermyte, Frederik

doi:10.3390/ijms22189927

Cited by 6 publications

(12 citation statements)

References 64 publications

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“…However, such organic consumption would reduce the degradation efficiency of diesels by competing with •OH. In addition, the intensity magnification of tyrosine-like protein after FT treatment may be ascribed to the hydrolysis of macromolecular proteins . On the other hand, after BP treatment, the content of FAL and protein-like substances (including tyrosine-like and tryptophan-like proteins) in BPS decreased, which was attributed to these substances having high reactivity in oxidation .…”

Section: Resultsmentioning

confidence: 97%

Unveiling Molecular Transformations of Soil Organic Matter after Remediation by Chemical Oxidation Based on ESI-FT-ICR-MS analysis

Wang

Wei

et al. 2023

ACS EST Eng.

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Remediation of soils contaminated with organic pollutants is often accomplished by chemical oxidation processes using oxidants such as persulfate or H 2 O 2 . However, it is unclear how different oxidants transform soil organic matter (SOM) and affect soil ecosystem services. Herein, two chemical oxidation technologies, Fenton reaction (FT) and base-activation of sodium persulfate (BP), were investigated to remediate diesel-polluted soils. The molecular transformation of SOM was analyzed using excitation−emission matrix fluorescence spectroscopy (EEM FS) and electrospray ionization coupled with Fourier transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS). Fulvic acid-like substances and lipids were consumed in both treatments, while the contents of lignin-like and tannin-like substances increased after BP treatment. The oxygen to carbon ratios (O/C), modified aromaticity index (AI mod ), and double bond equivalent (DBE) of SOM increased significantly in BP-treated soil, while these parameters decreased in FT-treated soil (FTS), suggesting the oxygen-containing, unsaturated and aromatic compounds were produced in BPS but removed in FTS. The increased cation exchange capacity (CEC) value (81.47 cmol/kg) and germination index of wheat seed (97%) for the SOM in BPS indicate the possible favorable effect of persulfate-based treatment on soil quality. Overall, this study advances mechanistic understanding of the effects of H 2 O 2 -and persulfate-based soil remediation technologies based on the molecular compositions of SOM and soil quality.

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Section: Resultsmentioning

confidence: 97%

Unveiling Molecular Transformations of Soil Organic Matter after Remediation by Chemical Oxidation Based on ESI-FT-ICR-MS analysis

Wang

Wei

et al. 2023

ACS EST Eng.

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“…In contrast, oxidizing 96 samples one by one using Fe(II)-EDTA/H 2 O 2 /ascorbate (e.g., ref ) would take hours. This length of time exceeds the stability of the Fe(II)-EDTA reagent (Figure S1I) and that of ascorbate and likely the endurance of all but the hardiest scientist. (iii) We have demonstrated that chemical generation of • OH is compatible with a range of solutes and conditions commonly used to analyze proteins (Figure S1).…”

Section: Discussionmentioning

confidence: 94%

“…That Fenton-generated • OH can be used for protein oxidative footprinting has been demonstrated. − These studies utilized the Tullius nucleic acid analysis approach of adding Fe(II)-EDTA, H 2 O 2 , and ascorbate to generate • OH in samples. While nucleic acid oxidative footprinting studies are typically conducted using a single radical dose, the importance of dose-dependent oxidation to protein analysis is well established. , We found that the Fe(II)-EDTA/H 2 O 2 /ascorbate cocktail does not support the reproducible dose-dependent generation of • OH required for reliable protein analysis.…”

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confidence: 99%

Systematic Fe(II)-EDTA Method of Dose-Dependent Hydroxyl Radical Generation for Protein Oxidative Footprinting

Chapman,

Paukner,

Leser

et al. 2023

Anal. Chem.

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Correlating the structure and dynamics of proteins with biological function is critical to understanding normal and dysfunctional cellular mechanisms. We describe a quantitative method of hydroxyl radical generation via Fe(II)-ethylenediaminetetraacetic acid (EDTA)catalyzed Fenton chemistry that provides ready access to protein oxidative footprinting using equipment commonly found in research and process control laboratories. Robust and reproducible dose-dependent oxidation of protein samples is observed and quantitated by mass spectrometry with as fine a single residue resolution. An oxidation analysis of lysozyme provides a readily accessible benchmark for our method. The efficacy of our oxidation method is demonstrated by mapping the interface of a RAS−monobody complex, the surface of the NIST mAb, and the interface between PRC2 complex components. These studies are executed using standard laboratory tools and a few pennies of reagents; the mass spectrometry analysis can be streamlined to map the protein structure with single amino acid residue resolution.

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“…Fits of the reaction profile using zeroth, first and second order kinetics (Figure S17; Figure S16; Figure S18). Ref [ 11 , 17 , 22 , 26 , 27 , 28 , 36 , 37 , 38 , 39 , 40 , 41 , 42 ] are cited in the Supplementary Materials.…”

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confidence: 99%

Detection and Verification of a Key Intermediate in an Enantioselective Peptide Catalyzed Acylation Reaction

2022

Self Cite

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Until now, the intermediate responsible for the acyl transfer of a highly enantioselective tetrapeptide organocatalyst for the kinetic resolution of trans-cycloalkane-1,2-diols has never been directly observed. It was proposed computationally that a π-methylhistidine moiety is acylated as an intermediate step in the catalytic cycle. In this study we set out to investigate whether we can detect and characterize this key intermediate using NMR-spectroscopy and mass spectrometry. Different mass spectrometric experiments using a nano-ElectroSpray Ionization (ESI) source and tandem MS-techniques allowed the identification of tetrapeptide acylium ions using different acylation reagents. The complexes of trans-cyclohexane-1,2-diols with the tetrapeptide were also detected. Additionally, we were able to detect acylated tetrapeptides in solution using NMR-spectroscopy and monitor the acetylation reaction of a trans-cyclohexane-1,2-diol. These findings are important steps towards the understanding of this highly enantioselective organocatalyst.

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Fenton-Chemistry-Based Oxidative Modification of Proteins Reflects Their Conformation

Cited by 6 publications

References 64 publications

Unveiling Molecular Transformations of Soil Organic Matter after Remediation by Chemical Oxidation Based on ESI-FT-ICR-MS analysis

Unveiling Molecular Transformations of Soil Organic Matter after Remediation by Chemical Oxidation Based on ESI-FT-ICR-MS analysis

Systematic Fe(II)-EDTA Method of Dose-Dependent Hydroxyl Radical Generation for Protein Oxidative Footprinting

Detection and Verification of a Key Intermediate in an Enantioselective Peptide Catalyzed Acylation Reaction

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