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1.
Sci Total Environ ; 838(Pt 1): 155790, 2022 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-35550890

RESUMO

The temporal evolution of molecular compositions and changes in structural features of Hillsboro Canal (Florida, USA) dissolved organic matter (DOM) was studied with an emphasis on nitrogen and sulfur containing molecules, after a 13 day time-series exposure to simulated sunlight. The Hillsboro Canal drains from the ridge and slough wetland environment underlain by peat soils from the northern extent of the Greater Everglades Ecosystem. The Hillsboro Canal-DOM was characterized by combining ultrahigh-resolution mass spectrometry (FT-ICR-MS), high-field nuclear magnetic resonance spectroscopy (1H NMR), size exclusion chromatography (SEC) with UV detection, and ultraviolet/visible (UV/vis) absorbance and excitation emission matrix (EEM) fluorescence spectroscopy. Size exclusion chromatography (SEC) demonstrated progressive depletion of higher mass molecules and a concomitant decrease of absorbance during photo-irradiation. NMR and FT-ICR-MS revealed nonlinear temporal evolution of DOM. In fact, FT-ICR-MS showed an initial depletion of supposedly chromophoric molecules often carrying major unsaturation accompanied by an uneven evolution of numbers of CHO, CHOS and CHNO compounds. While CHNO compounds continually increased throughout the entire photo-exposure time, CHO and CHOS compounds temporarily increased but declined after further light exposure. Progressive loss of highly unsaturated compounds was accompanied by production of low mass CHO and CHNO compounds with high O/C ratios. Area-normalized 1H NMR spectra of DOM in water and of the water insoluble fraction (~5%) in methanol revealed clear distinctions between irradiated and non-irradiated samples and congruent evolution of DOM structural features during irradiation, with more uniform trends in methanolic-DOM. Photoirradiation caused initial photoproduction of oxygenated aliphatic compounds, continued depletion of phenols and oxygenated aromatics, substantial change from initial natural product derived olefins to photoproduced olefins, and uneven evolution of carboxylated and alkylated benzene derivatives. This study demonstrates longer-term heteroatom-dependent photochemistry of DOM, which will affect the speciation of N and S heteroatoms, their connections to inorganic nutrients, and potentially their bioavailability.

2.
Metabolites ; 12(4)2022 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-35448510

RESUMO

White wine's oxidative stability after several years of bottle aging is synonymous to its organoleptic quality. In order to gain control over the cascade of chemical reactions that are implicated in that phenomenon, fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS)-based metabolomics and sensory evaluation were combined for the analysis of a vertical series of white wines from different vineyard plots. Data mining using supervised cluster analysis allowed the extraction of known and unknown sulfur- and nitrogen-containing molecular features, with oxidative stability molecular markers presenting an increased number of S and O atoms in their formulas. In their majority, S-containing molecular features possessed between 4 to ~12 O atoms, indicating the relatively higher importance of sulfonation reactions as opposed to dimerization reactions. Molecular networking, based on sulfonation reaction transformations, evidences the importance of hitherto unknown and/or minor sulfur dioxide binders (peptides, aldehydes, and polyphenols) on wine's oxidative stability.

3.
Anal Chem ; 94(15): 5953-5961, 2022 04 19.
Artigo em Inglês | MEDLINE | ID: mdl-35389626

RESUMO

Identification of chemically modified peptides in mass spectrometry (MS)-based glycation studies is a crucial yet challenging task. There is a need to establish a mode for matching tandem mass spectrometry (MS/MS) data, allowing for both known and unknown peptide glycation modifications. We present an open search approach that uses classic and modified peptide fragment ions. The latter are shifted by the mass delta of the modification. Both provide key structural information that can be used to assess the peptide core structure of the glycation product. We also leverage redundant neutral losses from the modification side chain, introducing a third ion class for matching referred to as characteristic fragment ions. We demonstrate that peptide glycation product MS/MS spectra contain multidimensional information and that most often, more than half of the spectral information is ignored if no attempt is made to use a multi-step matching algorithm. Compared to regular and/or modified peptide ion matching, our triple-ion strategy significantly increased the median interpretable fraction of the glycation product MS/MS spectra. For reference, we apply our approach for Amadori product characterization and identify all established diagnostic ions automatically. We further show how this method effectively applies the open search concept and allows for optimized elucidation of unknown structures by presenting two hitherto undescribed peptide glycation modifications with a delta mass of 102.0311 and 268.1768 Da. We characterize their fragmentation signature by integration with isotopically labeled glycation products, which provides high validity for non-targeted structure identification.


Assuntos
Peptídeos , Espectrometria de Massas em Tandem , Glicosilação , Íons , Fragmentos de Peptídeos , Peptídeos/química , Espectrometria de Massas em Tandem/métodos
4.
Rapid Commun Mass Spectrom ; 36(11): e9283, 2022 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-35229909

RESUMO

RATIONALE: Sugars are key molecules of life but challenging to detect via electrospray ionization mass spectrometry (ESI-MS). Unfortunately, sugars are challenging analytes for mass spectrometric methods due to their high gas-phase deprotonation energies and low gas-phase proton affinities which make them difficult to ionize in high abundance for MS detection. METHODS: Hydrogen-bond interactions in H2 PO4 - -saccharide anionic systems were studied both experimentally (via electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry, ESI-FT-ICR-MS) and computationally by several sophisticated density-functional theoretical methods (DFT and DFT-D3). RESULTS: The H2 PO4 - dopant boosts the detection of sugars up to 51-times in the case of sucrose and up to 263-times for glucose (at 0.1 ppm concentration level). H2 PO4 - binds toward sugar molecules with noticeably more hydrogen bonds than the established dopant chloride Cl- does, with increasing binding energies in the order: Monosaccharides < Trisaccharides < Disaccharides. Analysis of a complex oak plant sample revealed that NH4 H2 PO4 specifically labeled a diverse set of sugar-type plant metabolites in the form of [M + H2 PO4 ]- complexes. CONCLUSIONS: We reveal the mechanism of interaction of H2 PO4 - with different sugars and glycosylated organic compounds, which significantly enhances their ionization in mass spectrometry. A computational and experimental investigation is presented. A strong correlation between the MS signal intensities of detected [M + H2 PO4 ]- anions of different saccharides and their calculated dissociation enthalpies was revealed. Thus, the variation in MS signal intensities can be very well described to a large extent by the variation in calculated saccharide affinities toward the H2 PO4 - dopant anion, showing that DFT-D3 can very well describe experimental FT-ICR-MS observations.

5.
Anal Chem ; 94(14): 5474-5482, 2022 04 12.
Artigo em Inglês | MEDLINE | ID: mdl-35344349

RESUMO

Non-targeted metabolomics via high-resolution mass spectrometry methods, such as direct infusion Fourier transform-ion cyclotron resonance mass spectrometry (DI-FT-ICR MS), produces data sets with thousands of features. By contrast, the number of samples is in general substantially lower. This disparity presents challenges when analyzing non-targeted metabolomics data sets and often requires custom methods to uncover information not always accessible via classical statistical techniques. In this work, we present a pipeline that combines a convolutional neural network with traditional statistical approaches and an adaptation of a genetic algorithm. The developed method was applied to a lifestyle intervention cohort data set, where subjects at risk of type 2 diabetes underwent an oral glucose tolerance test. Feature selection is the final result of the pipeline, achieved through classification of the data set via a neural network, with a precision-recall score of over 0.9 on the test set. The features most relevant for the described classification were then chosen via a genetic algorithm. The output of the developed pipeline encompasses approximately 200 features with high predictive scores, providing a fingerprint of the metabolic changes in the prediabetic class on the data set. Our framework presents a new approach which allows to apply complex modeling based on convolutional neural networks for the analysis of high-resolution mass spectrometric data.


Assuntos
Diabetes Mellitus Tipo 2 , Humanos , Espectrometria de Massas/métodos , Metabolômica/métodos , Redes Neurais de Computação
6.
Metabolites ; 12(3)2022 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-35323678

RESUMO

Kombucha is a fermented beverage obtained through the activity of a complex microbial community of yeasts and bacteria. Exo-metabolomes of kombucha microorganisms were analyzed using FT-ICR-MS to investigate their interactions. A simplified set of microorganisms including two yeasts (Brettanomyces bruxellensis and Hanseniaspora valbyensis) and one acetic acid bacterium (Acetobacter indonesiensis) was used to investigate yeast-yeast and yeast-acetic acid bacterium interactions. A yeast-yeast interaction was characterized by the release and consumption of fatty acids and peptides, possibly in relationship to commensalism. A yeast-acetic acid bacterium interaction was different depending on yeast species. With B. bruxellensis, fatty acids and peptides were mainly produced along with consumption of sucrose, fatty acids and polysaccharides. In opposition, the presence of H. valbyensis induced mainly the decrease of polyphenols, peptides, fatty acids, phenolic acids and putative isopropyl malate and phenylpyruvate and few formulae have been produced. With all three microorganisms, the formulae involved with the yeast-yeast interactions were consumed or not produced in the presence of A. indonesiensis. The impact of the yeasts' presence on A. indonesiensis was consistent regardless of the yeast species with a commensal consumption of compounds associated to the acetic acid bacterium by yeasts. In detail, hydroxystearate from yeasts and dehydroquinate from A. indonesiensis were potentially consumed in all cases of yeast(s)-acetic acid bacterium pairing, highlighting mutualistic behavior.

7.
Biomedicines ; 10(3)2022 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-35327418

RESUMO

Glucotoxic metabolites and pathways play a crucial role in diabetic complications, and new treatment options which improve glucotoxicity are highly warranted. In this study, we analyzed bezafibrate (BEZ) treated, streptozotocin (STZ) injected mice, which showed an improved glucose metabolism compared to untreated STZ animals. In order to identify key molecules and pathways which participate in the beneficial effects of BEZ, we studied plasma, skeletal muscle, white adipose tissue (WAT) and liver samples using non-targeted metabolomics (NMR spectroscopy), targeted metabolomics (mass spectrometry), microarrays and mitochondrial enzyme activity measurements, with a particular focus on the liver. The analysis of muscle and WAT demonstrated that STZ treatment elevated inflammatory pathways and reduced insulin signaling and lipid pathways, whereas BEZ decreased inflammatory pathways and increased insulin signaling and lipid pathways, which can partly explain the beneficial effects of BEZ on glucose metabolism. Furthermore, lysophosphatidylcholine levels were lower in the liver and skeletal muscle of STZ mice, which were reverted in BEZ-treated animals. BEZ also improved circulating and hepatic glucose levels as well as lipid profiles. In the liver, BEZ treatment reduced elevated fumarate levels in STZ mice, which was probably due to a decreased expression of urea cycle genes. Since fumarate has been shown to participate in glucotoxic pathways, our data suggests that BEZ treatment attenuates the urea cycle in the liver, decreases fumarate levels and, in turn, ameliorates glucotoxicity and reduces insulin resistance in STZ mice.

8.
J Fungi (Basel) ; 8(2)2022 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-35205905

RESUMO

Copper-based preparations have been used for more than 100 years in viticulture to control downy mildew caused by Plasmopara viticola. LC2017, and a new low-copper-based formulation, has been developed to control grapevine trunk diseases (GTDs). Previous greenhouse studies showed the potential of LC2017 to control GTDs by both fungistatic and plant defense elicitor effects. Here, we further characterize the effects of LC2017 in the field determining its impact on: (i) incidence of Esca, (ii) the vine microbiome, (iii) the vine physiology and (iv) enological parameters of juices. We observed a progressive decrease of cumulate Esca incidence in treated vines over the years with annual fluctuation related to the known erratic emergence of GTD symptoms. Neither harmful effects of LC2017 on the vine microbiota, nor on vine physiology were observed (at both transcriptomic and metabolomic levels). Similarly, no impact of LC2017 was observed on the enological properties of berries except for sugar content in juice from esca-diseased vines. The most important result concerns the transcriptomic profiles: that of diseased and LC2017 treated vines differs from that of disease untreated ones, showing a treatment effect. Moreover, the transcriptomic profile of diseased and LC2017-treated vines is similar to that of untreated asymptomatic vines, suggesting control of the disease.

9.
Metabolites ; 12(2)2022 Jan 19.
Artigo em Inglês | MEDLINE | ID: mdl-35208168

RESUMO

Plants are continuously interacting with other organisms to optimize their performance in a changing environment. Mycorrhization is known to affect the plant growth and nutrient status, but it also can lead to adjusted plant defense and alter interactions with other trophic levels. Here, we studied the effect of Laccaria bicolor-mycorrhization on the poplar (Populus x canescens) metabolome and volatilome on trees with and without a poplar leaf beetle (Chrysomela populi) infestation. We analyzed the leaf and root metabolomes employing liquid chromatography-mass spectrometry, and the leaf volatilome employing headspace sorptive extraction combined with gas-chromatography-mass spectrometry. Mycorrhization caused distinct metabolic adjustments in roots, young/infested leaves and old/not directly infested leaves. Mycorrhization adjusted the lipid composition, the abundance of peptides and, especially upon herbivory, the level of various phenolic compounds. The greatest change in leaf volatile organic compound (VOC) emissions occurred four to eight days following the beetle infestation. Together, these results prove that mycorrhization affects the whole plant metabolome and may influence poplar aboveground interactions. The herbivores and the mycorrhizal fungi interact with each other indirectly through a common host plant, a result that emphasizes the importance of community approach in chemical ecology.

10.
Metabolites ; 12(2)2022 Feb 08.
Artigo em Inglês | MEDLINE | ID: mdl-35208234

RESUMO

Kombucha is a traditional fermented beverage obtained from the transformation of sugared black tea by a community of yeasts and bacteria. Kombucha production recently became industrialized, but its quality standards remain poorly defined. Metabolomic analyses were applied using FT-ICR-MS to characterize the impacts of production phases and the type of tea on the non-volatile chemical composition of kombucha. Independently from tea type, the first phase of acidification in open vessel was characterized by the release of gluconate and gallate from acetic acid bacteria metabolism and probably from polymeric polyphenols, respectively. The second phase of carbonation in closed vessel induced a consumption or transformation of oleic acid that could be consecutive of oxygen limitation. The first phase had the most impact on molecular diversity, but tea type mainly influenced the global composition in polyphenol profile. Black tea polyphenols were more impacted by microbial activity compared to green tea polyphenols.

11.
Metabolites ; 12(1)2022 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-35050158

RESUMO

Chronic respiratory diseases such as asthma are highly prevalent in industrialized countries. As cases are expected to rise, there is a growing demand for alternative therapies. Our recent research on the potential benefits of probiotics suggests that they could prevent and reduce the symptoms of many diseases by modulating the host immune system with secreted metabolites. This article presents the first steps of the research that led us to identify the immunoregulatory bioactivity of the amino acid d-Trp reported in our previous study. Here we analyzed the cell culture metabolic footprinting of 25 commercially available probiotic strains to associate metabolic pathway activity information with their respective immune modulatory activity observed in vitro. Crude probiotic supernatant samples were processed in three different ways prior to untargeted analysis in positive and negative ionization mode by direct infusion ESI-FT-ICR-MS: protein precipitation and solid phase extraction (SPE) using HLB and CN-E sorbent cartridges. The data obtained were submitted to multivariate statistical analyses to distinguish supernatant samples into the bioactive and non-bioactive group. Pathway analysis using discriminant molecular features showed an overrepresentation of the tryptophan metabolic pathway for the bioactive supernatant class, suggesting that molecules taking part in that pathway may be involved in the immunomodulatory activity observed in vitro. This work showcases the potential of metabolomics to drive product development and novel bioactive compound discovery out of complex biological samples in a top-down manner.

12.
Cell Death Differ ; 29(3): 670-686, 2022 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-34663908

RESUMO

Ferroptosis is an iron-dependent form of cell death driven by biochemical processes that promote oxidation within the lipid compartment. Calcium (Ca2+) is a signaling molecule in diverse cellular processes such as migration, neurotransmission, and cell death. Here, we uncover a crucial link between ferroptosis and Ca2+ through the identification of the novel tetraspanin MS4A15. MS4A15 localizes to the endoplasmic reticulum, where it blocks ferroptosis by depleting luminal Ca2+ stores and reprogramming membrane phospholipids to ferroptosis-resistant species. Specifically, prolonged Ca2+ depletion inhibits lipid elongation and desaturation, driving lipid droplet dispersion and formation of shorter, more saturated ether lipids that protect phospholipids from ferroptotic reactive species. We further demonstrate that increasing luminal Ca2+ levels can preferentially sensitize refractory cancer cell lines. In summary, MS4A15 regulation of anti-ferroptotic lipid reservoirs provides a key resistance mechanism that is distinct from antioxidant and lipid detoxification pathways. Manipulating Ca2+ homeostasis offers a compelling strategy to balance cellular lipids and cell survival in ferroptosis-associated diseases.


Assuntos
Fenômenos Bioquímicos , Ferroptose , Cálcio , Peroxidação de Lipídeos , Oxirredução , Fosfolipídeos
13.
Food Chem ; 374: 131618, 2022 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-34823930

RESUMO

Untargeted research on vapor arising during the thermal processing of food has so far focused on volatile aroma compounds. In this study, we present an oven atmosphere sampling strategy to trap headspace aerosols along with semi- and non-volatile molecules liberated during the baking of wheat bread rolls. The collected vapor condensate was analyzed for its molecular fingerprinting using direct infusion ultra-high resolution mass spectrometry. We detected up to 4,700 molecular species in a vapor sample from bread rolls baked at 230 °C for 15 min. Beyond the global profiling of the underlying matrix, our method can follow complex reaction cascades during the baking process, such as the formation of advanced glycation end-products like maltosine through the interface of trapped vapor. Further, process parameters such as baking temperature and duration were used to model the dynamic liberation of molecules to the oven atmosphere by a response surface methodology approach.


Assuntos
Pão , Produtos Finais de Glicação Avançada , Pão/análise , Espectrometria de Massas , Odorantes , Temperatura
15.
Front Chem ; 9: 788094, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34957049

RESUMO

Parkinson´s disease progression is linked to iron redox status homeostasis via reactive oxygen species (ROS) formation, and lipids are the primary targets of ROS. The determination of iron redox status in vivo is challenging and requires specific extraction methods, which are so far tedious and very time-consuming. We demonstrated a novel, faster, and less laborious extraction method using the chelator ethylene glycol l-bis(ß-aminoethyl ether)-N,N,N',N'-tetra acetic acid (EGTA) as a stabilizing agent and synthetic quartz beads for homogenization under an argon atmosphere. Additionally, we combined the metal extraction with a well-established lipid extraction protocol using methyl-tert-butyl ether (MTBE) to avoid the problems of lipid precipitation in frozen samples and to determine lipid profiles and metal species from the same batch. The nonextractable matrix, such as the debris, is removed by centrifugation and digested to determine the total metal content of the sample as well. Lipid profiling using RP-LC-MS demonstrated high accordance of the modified extraction method to the reference method, and the organic solvent does not affect the iron redox status equilibrium. Furthermore, rigorous testing demonstrated the stability of the iron redox status equilibrium during the extraction process, secured by complexation, inert atmosphere, fast preparation, and immediately deep frozen extracts.

16.
Cells ; 10(11)2021 10 20.
Artigo em Inglês | MEDLINE | ID: mdl-34831029

RESUMO

Background: Although several approaches have revealed much about individual factors that regulate pancreatic development, we have yet to fully understand their complicated interplay during pancreas morphogenesis. Gfi1 is transcription factor specifically expressed in pancreatic acinar cells, whose role in pancreas cells fate identity and specification is still elusive. Methods: In order to gain further insight into the function of this factor in the pancreas, we generated animals deficient for Gfi1 specifically in the pancreas. Gfi1 conditional knockout animals were phenotypically characterized by immunohistochemistry, RT-qPCR, and RNA scope. To assess the role of Gfi1 in the pathogenesis of diabetes, we challenged Gfi1-deficient mice with two models of induced hyperglycemia: long-term high-fat/high-sugar feeding and streptozotocin injections. Results: Interestingly, mutant mice did not show any obvious deleterious phenotype. However, in depth analyses demonstrated a significant decrease in pancreatic amylase expression, leading to a diminution in intestinal carbohydrates processing and thus glucose absorption. In fact, Gfi1-deficient mice were found resistant to diet-induced hyperglycemia, appearing normoglycemic even after long-term high-fat/high-sugar diet. Another feature observed in mutant acinar cells was the misexpression of ghrelin, a hormone previously suggested to exhibit anti-apoptotic effects on ß-cells in vitro. Impressively, Gfi1 mutant mice were found to be resistant to the cytotoxic and diabetogenic effects of high-dose streptozotocin administrations, displaying a negligible loss of ß-cells and an imperturbable normoglycemia. Conclusions: Together, these results demonstrate that Gfi1 could turn to be extremely valuable for the development of new therapies and could thus open new research avenues in the context of diabetes research.


Assuntos
Proteínas de Ligação a DNA/deficiência , Diabetes Mellitus/metabolismo , Diabetes Mellitus/prevenção & controle , Fatores de Transcrição/deficiência , Células Acinares/citologia , Células Acinares/metabolismo , Amilases/metabolismo , Animais , Diferenciação Celular/genética , Proliferação de Células/genética , Proteínas de Ligação a DNA/genética , Proteínas de Ligação a DNA/metabolismo , Diabetes Mellitus/genética , Modelos Animais de Doenças , Regulação da Expressão Gênica , Grelina/metabolismo , Proteínas de Homeodomínio/metabolismo , Hiperglicemia/complicações , Hiperglicemia/genética , Integrases/metabolismo , Camundongos Transgênicos , Mutação/genética , Pâncreas/metabolismo , Fatores de Transcrição/genética , Fatores de Transcrição/metabolismo
17.
Sci Rep ; 11(1): 21543, 2021 11 02.
Artigo em Inglês | MEDLINE | ID: mdl-34728655

RESUMO

The preservation of biosignatures on Mars is largely associated with extensive deposits of clays formed under mild early Noachian conditions (> 3.9 Ga). They were followed by widespread precipitation of acidic sulfates considered adverse for biomolecule preservation. In this paper, an exhaustive mass spectrometry investigation of ferric subsurface materials in the Rio Tinto gossan deposit (~ 25 Ma) provides evidence of well-preserved molecular biosignatures under oxidative and acidic conditions. Time of flight secondary ion mass spectrometry (ToF-SIMS) analysis shows a direct association between physical-templating biological structures and molecular biosignatures. This relation implies that the quality of molecular preservation is exceptional and provides information on microbial life formerly operating in the shallow regions of the Rio Tinto subsurface. Consequently, low-pH oxidative environments on Mars could also record molecular information about ancient life in the same way as the Noachian clay-rich deposits.

18.
Cell Metab ; 33(12): 2355-2366.e8, 2021 12 07.
Artigo em Inglês | MEDLINE | ID: mdl-34847376

RESUMO

Hexokinases (HK) catalyze the first step of glycolysis limiting its pace. HK2 is highly expressed in gut epithelium, contributes to immune responses, and is upregulated during inflammation. We examined the microbial regulation of HK2 and its impact on inflammation using mice lacking HK2 in intestinal epithelial cells (Hk2ΔIEC). Hk2ΔIEC mice were less susceptible to acute colitis. Analyzing the epithelial transcriptome from Hk2ΔIEC mice during colitis and using HK2-deficient intestinal organoids and Caco-2 cells revealed reduced mitochondrial respiration and epithelial cell death in the absence of HK2. The microbiota strongly regulated HK2 expression and activity. The microbially derived short-chain fatty acid (SCFA) butyrate repressed HK2 expression via histone deacetylase 8 (HDAC8) and reduced mitochondrial respiration in wild-type but not in HK2-deficient Caco-2 cells. Butyrate supplementation protected wild-type but not Hk2ΔIEC mice from colitis. Our findings define a mechanism how butyrate promotes intestinal homeostasis and suggest targeted HK2-inhibition as therapeutic avenue for inflammation.


Assuntos
Colite , Hexoquinase , Animais , Células CACO-2 , Morte Celular/fisiologia , Colite/metabolismo , Colite/microbiologia , Células Epiteliais/metabolismo , Hexoquinase/metabolismo , Histona Desacetilases/metabolismo , Humanos , Camundongos , Mitocôndrias/metabolismo , Proteínas Repressoras/metabolismo
19.
Front Chem ; 9: 715372, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34354980

RESUMO

Here, we report a non-targeted analytical approach to investigate the influence of different starch sources on the metabolic signature in the final beer product. An extensive sample set of commercial beers brewed with barley, wheat, corn and/or rice were analyzed by both direct infusion Fourier transform ion cyclotron mass spectrometry (DI-FTICR MS, 400 samples) and UPLC-ToF-MS (100 samples). By its unrivaled mass resolution and accuracy, DI-FTICR-MS was able to uncover the compositional space of both polar and non-polar metabolites that can be traced back to the use of different starch sources. Reversed phase UPLC-ToF-MS was used to access information about molecular structures (MS2-fragmentation spectra) and isomeric separation, with a focus on less polar compounds. Both analytical approaches were able to achieve a clear statistical differentiation (OPLS-DA) of beer samples and reveal metabolic profiles according to the starch source. A mass difference network analysis, applied to the exact marker masses resolved by FTICR, showed a network of potential secondary metabolites specific to wheat, corn and rice. By MS2-similarity networks, database and literature search, we were able to identify metabolites and compound classes significant for the use of the different starch sources. Those were also found in the corresponding brewing raw materials, confirming the potential of our approach for quality control and monitoring. Our results also include the identification of the aspartic acid-conjugate of N-ß-D-glucopyranosyl-indole-3-acetic acid as a potential marker for the use of rice in the brewing industry regarding quality control and food inspection purposes.

20.
Metabolites ; 11(7)2021 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-34202850

RESUMO

Our skin influences our physical and mental health, and its chemical composition can reflect environmental and disease conditions. Therefore, through sampling the skin metabolome, we can provide a promising window into the mechanisms of the body. However, the broad application of skin metabolomics has recently been hampered by a lack of easy and widely applicable sampling methods. Here, we present a novel rapid, simple, and, most importantly, painless and non-invasive sampling technique suitable for clinical studies of fragile or weakened skin. The method is called WET PREP and is simply a lavage of the skin which focuses on capturing the metabolome. We systematically evaluate WET PREPs in comparison with the non-invasive method of choice in skin metabolomics, swab collection, using ultra-performance liquid chromatography coupled to mass spectrometry (UPLC-MS2) on two complementary chromatographic columns (C18 reversed phase and hydrophilic interaction chromatography). We also integrate targeted analyses of key metabolites of skin relevance. Overall, WET PREP provides a strikingly more stable shared metabolome across sampled individuals, while also being able to capture unique individual metabolites with a high consistency in intra-individual reproducibility. With the exception of (phospho-)lipidomic studies, we recommend WET PREPs as the preferred skin metabolome sampling technique due to the quick preparation time, low cost, and gentleness for the patient.

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