Selenium Decipher: Trapping of Native Selenomethionine-Containing Peptides in Selenium-Enriched Milk and Unveiling the Deterioration after Ultrahigh-Temperature Treatment.

Selenopeptide identification relies on databases to interpret the selenopeptide spectra. A common database search strategy is to set selenium as a variable modification instead of sulfur on peptides. However, this approach generally detects only a fraction of selenopeptides. An alternative approach, termed Selenium Decipher, is proposed in the present study. It involves identifying collision-induced dissociation-cleavable selenomethionine-containing peptides by iteratively matching the masses of seleno-amino acids in selenopeptide spectra. This approach uses variable-data-independent acquisition (vDIA) for peptide detection, providing a flexible and customizable window for secondary mass spectral fragmentation. The attention mechanism was used to capture global information on peptides and determine selenomethionine-containing peptide backbones. The core structure of selenium on selenomethionine-containing peptides generates a series of fragment ions, namely, C3H7Se+, C4H10NSe+, C5H7OSe+, C5H8NOSe+, and C7H11N2O2Se+, with known mass gaps during higher-energy collisional dissociation (HCD) fragmentation. De-selenium spectra are generated by removing selenium originating from selenium replacement and then reassigning the precursors to peptides. Selenium-enriched milk is obtained by feeding selenium-rich forage fed to cattle, which leads to the formation of native selenium through biotransformation. A novel antihypertensive selenopeptide Thr-Asp-Asp-Ile-SeMet-Cys-Val-Lys TDDI(Se)MCVK was identified from selenium-enriched milk. The selenopeptide (IC50 = 60.71 µM) is bound to four active residues of the angiotensin-converting enzyme (ACE) active pocket (Ala354, Tyr523, His353, and His513) and two active residues of zinc ligand (His387 and Glu411) and exerted a competitive inhibitory effect on the spatial blocking of active sites. The integration of vDIA and the iteratively matched seleno-amino acids was applied for Selenium Decipher, which provides high validity for selenomethionine-containing peptide identification.

3-Monochloropropane-1,2-diol reduced bioaccessibility of sn-2 palmitate via binding with pancreatic lipase in infant formula during gastrointestinal digestion.

Infant formula contains 3-monochloropropane-1,2-diol esters (3-MCPDE), which are formed during the deodorization step of vegetable oil refining. The European Food Safety Authority stated that 3-MCPDE can be hydrolyzed in the gastrointestinal tract to free-form 3-monochloropropane-1,2-diol (3-MCPD), which has potential toxicity and can be rapidly absorbed. Evaluating the effect of 3-MCPD on nutrition absorption is a prerequisite for establishing effective management strategies. A total of 66 crucial lipid molecules associated with 3-MCPD were identified based on debiased sparse partial correlation analysis. 3-MCPD affected triglyceride hydrolyzation and increased the concentration of undigested sn-2 palmitate (9.57 to 17.06 mg kg-1). 3-Monochloropropane-1,2-diol reduced the bioaccessibility of fatty acids, and more short- (31.42 to 58.02 mg kg-1) and medium-chain fatty acids (17.03 to 26.43 mg kg-1) remained unabsorbed. Lipidomic profiles of infant formula models spiked with different 3-MCPDE levels were investigated, and the results were consistent with the experiments with the commercial formula indicating lipid alteration was mainly affected by the digestive 3-MCPD. The formation of 3-MCPD ester-pancreatic lipase with the binding energy of -4.9 kcal mol-1 was more stable than triglyceride-pancreatic lipase (-4.0 kcal mol-1), affecting triglyceride hydrolyzation. 3-Monochloropropane-1,2-diol was bound to Glu13 and Asp331 residues of the pancreatic lipase via hydrogen bonds, which resulted in a conformational change of pancreatic lipase and spatial shielding effect. The existence of the spatial-shielding effect reduced the accessibility of pancreatic lipase and further affected triglyceride hydrolyzation. These findings indicated that 3-MCPD obstructed nutrient acquisition and laid the foundation for the subsequent nutrition enhancement design.

Multimodal deep learning as a next challenge in nutrition research: tailoring fermented dairy products based on cytidine diphosphate-diacylglycerol synthase-mediated lipid metabolism.

Deep learning is evolving in nutritional epidemiology to address challenges including precise nutrition and data-driven disease modeling. Fermented dairy products consumption as the implementation of specific dietary priority contributes to a lower risk of all-cause mortality, cardiovascular disease, and obesity. Various lipid types play different roles in cardiometabolic health and fermentation process changes the lipid profile in dairy products. Leveraging the power of multiple biological datasets can provide mechanistic insights into how proteins impact lipid pathways, and establish connections among fermentation-lipid biomarkers-protein. The recent leap of deep learning has been performed in food category recognition, agro-food freshness detection, and food flavor prediction and regulation. The proposed multimodal deep learning method includes four steps: (i) Forming data matrices based on data generated from different omics layers. (ii) Decomposing high-dimensional omics data according to self-attention mechanism. (iii) Constructing View Correlation Discovery Network to learn the cross-omics correlations and integrate different omics datasets. (iv) Depicting a biological network for lipid metabolism-centered quantitative multi-omics data analysis. Relying on the cytidine diphosphate-diacylglycerol synthase-mediated lipid metabolism regulates the glycerophospholipid composition of fermented dairy effectively. Innovative processing strategies including ohmic heating and pulsed electric field improve the sensory qualities and nutritional characteristics of the products.

Spatiotemporal Variation of Residual Cortisol Obstructs Nutrient Acquisition in Animal-Derived Foods by Perturbing Glycerophospholipid Metabolism.

Cortisol is inevitably secreted by pigs due to the physical and psychological stressors produced by mixed group transportation and preslaughter handling. Accumulated cortisol in animal tissues enters the human body through the food chain and entails potential risks to human health. An integrated lipidome and proteome analysis was conducted to investigate the effect of the spatiotemporal variation of residual cortisol on nutrient acquisition in pork. A total of 55 crucial lipid molecules associated with cortisol residue were identified based on debiased sparse partial correlation analysis. Label-free proteomics was applied to screen 58 differentially abundant proteins (including phospholipase A2, lysophosphatidylcholine acyltransferase, and CTP:phosphocholine cytidylyltransferase), indicating that cortisol residue perturbed the glycerophospholipid biosynthetic process and glycerophospholipid metabolic process. Cortisol induced downregulations of cPLA2 encoding genes and decreased phospholipase A2 activity, resulting in the bioaccumulation of phosphatidylethanolamine (from 36.86 to 43.18 mg kg-1). Cortisol increased the activity of CTP:phosphocholine cytidylyltransferase by improving the availability of fatty acids and aggregating the inactive L-form (lipid-independent form) to the active H-form (lipid-associated form). The metabolic pathways perturbed by cortisol resulted in phosphatidylcholine degradation (from 93.73 to 58.28 mg kg-1) and lysophosphatidylcholine accumulation (from 3.39 to 5.16 mg kg-1). These findings indicated that cortisol residue deteriorated meat quality and obstructed nutrient acquisition in animal-origin foods.

Naturally forming benzoic acid orientates perilipin to facilitate glyceride-type polyunsaturated fatty acid degradation via fermentation behavior.

Naturally forming benzoic acid in fermented dairy products accumulates in organisms and biomagnifies through collateral transport. The association between benzoic acid agglomeration and susceptible lipid nutrients remains obscure. Horizontal analysis of lipidomic alteration in response to benzoic acid was conducted and the spatially proteomic map was constructed using label-free quantitative proteomics. From synergistic integration of multi-omics in benzoic acid accumulated fermented goat milk model, the biological processes of significant proteins mostly focused on glyceride-type polyunsaturated fatty acids degradation (143.818 ± 0.51 mg/kg to 104.613 ± 0.29 mg/kg). As a physiological barrier shield, perilipin, which is coated on the surface of lipid droplets, protects triacylglycerols from cytosolic lipases, thus preventing triglyceride hydrolysis. The expression of perilipin decreased by 90% compared with the control group, leading to the decrease of triglycerides. Benzoic acid suppressed phosphatidylethanolamines and phosphatidylcholines synthesis by attenuating choline phosphotransferase and ethanolamine phosphotransferase. Less diglyceride generated by the dephosphorylation of phosphatidic acid entered choline phosphotransferase and ethanolamine phosphotransferase-mediated glycerophospholipid metabolisms. Fermentation of goat milk at a low temperature and less incubation time leads to the production of less benzoic acid and mitigation of lipid nutrient loss. The present study delineated the molecular landscape of fermented goat milk containing endogenous benzoic acid and further dissected the trajectory guiding lipid alteration to advance control of benzoic acid residue.

Magnetic field-driven biochemical landscape of browning abatement in goat milk using spatial-omics uncovers.

Influence of magnetic field (MF) treatment on the glycation of goat milk proteins is yet to be elucidated. Proteomic and metabolomic analyses of brown goat milk samples with and without MF treatment were performed. Assessed glycation degree and structural modification of proteins explained that MF treatment dramatically down-regulated the glycation of brown goat milk protein, possibly due to the aggregation behavior induced by MF treatment, which consumed additional glycation sites as well as altered their accessibility and preference. Integrated datasets uncovered that the energy metabolism-related biological events including carbohydrate metabolism, glycerophospholipid metabolism, TCA cycle may mainly account for the browning abatement mechanism of MF. In addition, MF treatment enhanced both the quality and flavor of brown goat milk. This study suggests the feasibility of MF treatment to reduce glycation in brown goat milk for producing high-quality dairy ingredients and products.

Quantitative fusion omics reveals that refrigeration drives methionine degradation through perturbing 5-methyltetrahydropteroyltriglutamate-homocysteine activity.

Postharvest senescence and quality deterioration of fresh tea leaves occurred due to the limitation of processing capacity. Refrigerated storage prolongs the shelf life of fresh tea. In this study, quantitative fusion omics delineated the translational landscape of metabolites and proteins in time-series (0-12 days) refrigerated tea by UHPLC-Q-Orbitrap HRMS. Accurate quantification results showed the content of amino acids, especially l-theanine, decreased with the lengthening of the storage duration (15.57 mg g-1 to 7.65 mg g-1) driven by theanine synthetase. Downregulation of enzyme 5-methyltetrahydropteroyltriglutamate-homocysteine methyltransferase expression led to methionine degradation (6.29 µg g-1 to 1.78 µg g-1). Refrigerated storage inhibited serine carboxypeptidase-like acyltransferases activity (59.49 % reduction in 12 days) and induced the polymerization of epicatechin and epigallocatechin and generation of procyanidin dimer and δ-type dehydrodicatechin, causing the manifestation of color deterioration. A predictive model incorporating zero-order reaction and Arrhenius equation was constructed to forecast the storage time of green tea.

Hydrocortisone-Containing Animal-Derived Food Intake Affects Lipid Nutrients Utilization.

SCOPE: As the tremendous increases in consumption of animal-derived food, endogenous hydrocortisone migrating along the food chain to organism arouses extensive attention. This study aims to investigate the cumulative impacts of dietary hydrocortisone intake and mechanistic understanding on metabolism of lipid nutrients. METHODS AND RESULTS: A total of 120 porcine muscles samples with different concentrations of hydrocortisone are collected at three time points. An operational food chain simulation framework is constructed and 175 lipid molecules are identified by UHPLC-Q-Orbitrap HRMS. Compared to the control group, 66 lipid molecules are significantly different, including 17 triglycerides and 31 glycerophospholipids. Integrated analyses of lipidomics and proteomics indicate that hydrocortisone promotes adipose triglyceride lipase and hormone sensitive lipase activity to precondition for triglycerides hydrolysis. Quantitative lipidomics analysis shows the presence of hydrocortisone decreases the concentration of docosahexaenoic acid (3.66 ± 0.15-3.09 ± 0.12 mg kg-1 ) and eicosapentanoic acid (0.54 ± 0.09-0.48 ± 0.06 mg kg-1 ). A noteworthy increase of most saturated triglycerides concentration with the prolonging of time is observed. CONCLUSIONS: Hydrocortisone originating from animal-derived food induces glycerophospholipids degradation and triglycerides hydrolysis through promoting adipose triglyceride lipase, hormone sensitive lipase, and phosphoglycerate kinase activity and further intervenes lipid nutrients utilization.

Monitoring contamination of perchlorate migrating along the food chain to dairy products poses risks to human health.

Assessments of human exposure to sodium perchlorate via dairy sources are limited. The current study applied untargeted metabolomics (LOD, 1.08-35.60 µg L-1; LOQ, 2.54-90.58 µg L-1; RSD < 6.2%) and proteomics methods by UHPLC-Q-Orbitrap HRMS to investigate the metabolic pathways and nutritional quality of goat milk contaminated with sodium perchlorate. Specifically, 11 metabolites including lactose (from 2.01 to 0.58 mg L-1), adenosine 5'-monophosphate (from 1.23 to 0.45 mg L-1), hypoxanthine (from 0.63 to 0.08 mg L-1), etc. and 3 crucial enzymes include α-lactalbumin, xanthine dehydrogenase and creatine kinase related to the quality traits of goat milk after sodium perchlorate treatment. Overall, except for spermidine, other related metabolites significantly decreased with the increase of sodium perchlorate concentration 0-160 µg L-1 and storage time (4-12 h). Collectively, we provide previously uncharacterized goat milk nutritional quality degradation mechanism induced by sodium perchlorate and a reference to ensure its safe use in human health.

UHPLC-Q-Orbitrap-based lipidomics reveals molecular mechanism of lipid changes during preservatives treatment of Hengshan goat meat sausages.

As preservative are extensively applied to prevent the quality degradation of Hengshan goat meat sausages, safety assessment based on lipid and elucidation of dynamic change mechanism is urgently needed. The effect of preservatives on lipidome profiles of sausages was investigated using UHPLC-Q-Orbitrap. Totally, 9 subclasses of 70 characteristic lipids (Cer, DG, LPC, PC, PE, PI, PS, SM, TG) were quantified accurately (LOD with 0.68-2.96 µg kg-1, LOQ with 2.25-9.79 µg kg-1, RSD < 3%). The decrease of TG concentration was the most significant, from 1072.43 mg kg-1 in preservative-free samples to 838.53, 786.41 and 681.35 mg kg-1 in natamycin, potassium sorbate and sodium diacetate treated samples, respectively. With regard to preservation and nutrition, natamycin was a potential preservative than two other preservatives. Significant lipid variables were primarily associated with glycerophospholipid and sphingolipid metabolism. Integration of both techniques provided a guide for meat industries to control spoilage with innovative strategies.

Irisin Attenuates Oxidative Stress, Mitochondrial Dysfunction, and Apoptosis in the H9C2 Cellular Model of Septic Cardiomyopathy through Augmenting Fundc1-Dependent Mitophagy.

In the present study, we used lipopolysaccharide- (LPS-) stimulated H9C2 cardiomyocytes to investigate whether irisin treatment attenuates septic cardiomyopathy via Fundc1-related mitophagy. Fundc1 levels and mitophagy were significantly reduced in LPS-stimulated H9C2 cardiomyocytes but were significantly increased by irisin treatment. Irisin significantly increased ATP production and the activities of mitochondrial complexes I and III in the LPS-stimulated cardiomyocytes. Irisin also improved glucose metabolism and significantly reduced LPS-induced levels of reactive oxygen species by increasing the activities of antioxidant enzymes, glutathione peroxidase (GPX), and superoxide dismutase (SOD), as well as levels of reduced glutathione (GSH). TUNEL assays showed that irisin significantly reduced LPS-stimulated cardiomyocyte apoptosis by suppressing the activation of caspase-3 and caspase-9. However, the beneficial effects of irisin on oxidative stress, mitochondrial metabolism, and viability of LPS-stimulated H9C2 cardiomyocytes were abolished by silencing Fundc1. These results demonstrate that irisin abrogates mitochondrial dysfunction, oxidative stress, and apoptosis through Fundc1-related mitophagy in LPS-stimulated H9C2 cardiomyocytes. This suggests irisin is a potentially useful treatment for septic cardiomyopathy, though further investigations are necessary to confirm our findings.

Effect of nisin and potassium sorbate additions on lipids and nutritional quality of Tan sheep meat.

Nisin and potassium sorbate as preservatives are used in a broad range of meat. A lipidomic evaluation was performed on Tan sheep meat treated by two types of preservatives. The addition of potassium sorbate resulted in higher lipid losses compared with nisin treatment. Furthermore, 106 significant lipids of 12 lipid classes (PC, PS, LPS, LPC, PE, PI, LPE, TG, Cer, DG, SM, Sph) with variable importance in projection scores greater than 1.0 were detected and qualified to distinguish different preservatives added meat using UHPLC-Q-Orbitrap MS/MS. LOD and LOQ were 0.12-0.32 µg kg-1 and 0.35-0.89 µg kg-1, indicating high sensitivity and excellent analytical characteristics in the study. Nisin was confirmed to be the better preservative for prolonging the shelf life of Tan sheep meat while reducing the loss of nutrients. These results could provide a strong cornerstone for future research on preservatives in meat products.

UHPLC-Q-Orbitrap HRMS-based quantitative lipidomics reveals the chemical changes of phospholipids during thermal processing methods of Tan sheep meat.

Thermal processing affects the lipid compositions of meat products. The study determined the effects of boiled, steamed and roasted processing methods on the lipidomics profiles of Tan sheep meat with a validated UPLC-Q-Orbitrap HRMS combined lipid screening strategy method. Combined with sphingolipid metabolism, the boiled approach was the suitable choice for atherosclerosis patients for more losses of sphingomyelin than ceramide in meat. The similarly less losses of phosphatidylcholine and lysophosphatidylcholine showed in glycerophospholipid metabolism implied that steamed Tan sheep meat was more suitable for the populations of elderly and infants. Furthermore, a total of 90 lipids with significant difference (VIP > 1) in 6 lipid subclasses (sphingomyelin, ceramide, lysophosphatidylcholine, phosphatidylcholine, phosphatidylethanolamines, triacylglycerol,) were quantified among raw and three types of thermal processed Tan sheep meat, further providing useful information for identification of meat products with different thermal processing methods (LOD with 0.14-0.31 µg kg-1, LOQ with 0.39-0.90 µg kg-1).

Molecular mechanism of lipid transformation in cold chain storage of Tan sheep.

Cold chain (-20 °C) is one of the main transportation methods for storage of Tan sheep products. Lipids (66) in seven subclasses involved in sphingolipid, glycerophospholipid and fatty acid degradation metabolism were quantified in Tan sheep under cold chain storage, including fatty acyl carnitines, phosphatidylcholine (PC), lysophosphatidylcholine (LPC), phosphatidylethanolamine (PE), ceramides, sphingomyelin (SM) and lysophosphatidylethanolamine (LPE). Lipid transformation and molecular mechanism analyzed using fragmentation mechanisms and UHPLC-Q-Orbitrap MS/MS combined with lipidomics approaches determined transient increases of certain PC, PE and fatty acyl carnitine during the first 12 days of cold storage, subsequent declines of SM, PC, PE and fatty acyl carnitine, as well as increases of ceramide, LPC and LPE (24 days). These results offered insights into lipid transformation and quality of Tan sheep during cold chain storage.