This study tackled mislabeling fraud in vegetable oils, driven by price disparities and profit motives, by developing an approach combining desorption electrospray ionization mass spectrometry (DESI-MS) with a shallow convolutional neural network (SCNN). The method was designed to characterize lipids and distinguish between nine vegetable oils: corn, soybean, peanut, sesame, rice bran, sunflower, camellia, olive, and walnut oils. The optimized DESI-MS method enhanced the ionization of non-polar glycerides and detected ion adducts like [TG + Na]+, [TG + NH4]+. This process identified 53 lipid peaks, forming a robust lipid fingerprint for each oil type. An SCNN model was developed using fingerprints, achieving an impressive classification accuracy of 98.5 +/- 2.2 %. The integration of DESI-MS with SCNN provides a fast and reliable tool for identifying and classifying vegetable oils, thereby reducing mislabeling fraud and assuring oil quality. By enabling accurate authentication, it contributes to improved transparency and integrity in food labeling and quality control practices.

Atherosclerosis is a primary cause of cardiovascular disease, straining healthcare systems. Dendrobium officinale, a widely used food-medicine homology, has demonstrated anti-atherosclerotic (anti-AS) properties, with other species listed in pharmacopoeias exhibiting similar effects. However, their efficacy varies, and the impact of interspecies variations on compounds and mechanisms in Dendrobium’s anti-AS effects remains unclear. This study aimed to explore the anti-AS compounds and mechanisms across various Dendrobium species. The chemical composition of D. fimbriatum, D. officinale, D. devonianum, D. gratiosissimum, and D. catenatum was analyzed using UPLC-Q-Exactive Orbitrap MS. Network pharmacology predicted the pharmacological basis and molecular mechanisms. Molecular docking experiments assessed the binding affinity of the identified compounds with target proteins. A total of 12 different and 65 common components were identified. Key therapeutic targets included SRC, STAT3, and PIK3CA, along with relevant signaling pathways linked to AS prevention. The study provides insights into interspecies differences in Dendrobium’s anti-AS properties.

Temperature fluctuations occurring during the cold chain logistics of salmon contribute to lipid oxidation. This study aimed to simulate cold chain interruption through freeze-thaw operations and evaluate the lipidomics data from salmon samples subjected to different numbers of freeze-thaw cycles by using rapid evaporative ionization mass spectrometry (REIMS) combined with an intelligent surgical knife (iKnife). The results indicated significant differences in the relative abundance of characteristic ions among the samples (p < 0.05). A total of 34 ions with variable importance for the projection values >= 1 were identified as potential biomarkers, including m/z 719.4233 ([PCC36:5-NH(CH3)(3)](-)), m/z 337.3134 ([FA(C22:1)](-)), m/z 720.4666 ([PEC35:6-H](-)), m/z 309.2780 ([FA(C20:1)](-)), m/z 777.4985 ([PCC40:4-NH(CH3)(3)](-)), m/z 745.4421 ([PCC38:6-NH(CH3)(3)](-)/[PEC38:6-NH3](-)), m/z 747.4665 ([PCC38:5-NH(CH3)(3)](-)/[PEC38:5-NH3](-)), etc. The degree of lipid oxidation was found to be associated with the number of freeze-thaw cycles, exhibiting the most significant alterations in the relative abundance of lipid ions in the 8T samples. Additionally, sensory evaluation by the CIE-L*a*b* method and volatile analysis by headspace solid-phase microextraction gas chromatography-mass spectrometry demonstrated significant differences (p < 0.05) in color and odor among the salmon samples, with a correlation to the number of freeze-thaw cycles. The primary compounds responsible for alterations in salmon odor were aldehydes with lower odor thresholds. In summary, the iKnife-REIMS method accurately differentiated salmon muscle tissues based on varying levels of lipid oxidation, thus expanding the application of REIMS.

Paralytic shellfish poisoning (PSP) is the most widespread and harmful form of shellfish poisoning with high mortality rate. In this study, a combined desorption electrospray ionization mass spectrometry (DESI-MS) and ultra -performance liquid chromatography triple quadrupole mass spectrometry (UPLC-QqQ/MS) method was established for the detection of PSPs in urine. The method was optimized using a spray solution of methanol and water (1:1, v/v) containing 0.1 % FA, at a flow rate of 2.5 mu L & sdot;min-1 and an applied voltage of 3 kV. The limit of detection (LOD) for PSPs detection by DESI-MS was in the range of 87-265 mu g & sdot;L-1, which basically meets the requirements for the rapid screening of PSPs. The LOD for UPLC-QqQ/MS was in the range of 2.2-14.9 mu g & sdot;L- 1, with a limit of quantification (LOQ) of 7.3-49.7 mu g & sdot;L-1, thus fulfilling the quantitative demand for PSPs in urine. Finally, after spiking the urine samples of six volunteers with PSPs to a concentration of 100 mu g & sdot;L-1, DESI-MS successfully and efficiently detected the positive samples. Subsequently, UPLC-QqQ/MS was employed for precise quantification, yielding results in the range of 84.6-95.1 mu g & sdot;L-1. The experimental findings demonstrated that the combination of DESI-MS and UPLC-QqQ/MS enables high -throughput, rapid screening of samples and accurate quantification of positive samples, providing assurance for food safety and human health.

Larimichthys crocea (LYC) holds significant economic value as a marine fish species. However, inaccuracies in labeling its origin can adversely affect consumer interests. Herein, a laser assisted rapid evaporative ionization mass spectrometry (LA-REIMS) and machine learning (ML) was developed for geographical authentication. When compared to iKnife, the LA demonstrated to be superior owing to reduced thermal damage to sample tissue, enhanced automation, and ease of use. Analysis of LYC from six distinct geographical origins across China revealed a total of 798 ions, which were then subjected to six classifiers to establish ML models. Following hyperparameter optimization and feature engineering, the Chi2(15%)-KNN model exhibited the highest training and testing accuracy, achieving 98.4 +/- 0.9% and 98.5 +/- 1.4%, respectively. This LA-REIMS/ML methodology offers a rapid, accurate, and intelligent solution for tracing the origin of LYC, thereby providing valuable technical support for the establishment of traceability systems in the aquatic product industry.

Antarctic krill oil (AKO) possesses potent bioactivities but has limited applications in the food industry due to its poor stability, strong off-flavor, and low bioavailability of contained astaxanthin. In this study, Antarctic krill protein isolate (AKPI) was separated from processing by-product of krill and utilized as a novel wall material via complexing it with gum Arabic (GA) to improve the limitations of AKO. The strong complex coacervation reaction between AKPI and GA was occurred at the pH of 3.8 and the ratioAKPI-to-GA of 3:1, while electrostatic interaction and hydrogen-bond interaction were determined to be the main driving forces of such reaction. The ratiowall-to-core was confirmed as 1:0.75 after comprehensively assessing the effect of AKO content on the various properties of AKPI-GA coacervated microcapsules, while the wall material concentration and pH were optimized at 1 % and 3.8, respectively. The obtained solid AKO microcapsules exhibited the encapsulation efficiency of 80.22 %. AKPI-GA coacervated microcapsules extremely masked the odor of AKO and achieved the controlled-release of AKO in the gastrointestinal tract. Meanwhile, the encapsulated AKO displayed higher astaxanthin retention and oxidative stability compared with non-encapsulated AKO during storage.

Freezing is one of the most commonly used preservation methods for Bluefin tuna (Thunnus orientalis). However, repeated freezing and thawing would inevitably occur due to the temperature fluctuation, leading to the microstructure damage, lipid oxidation and protein integrity decline of tuna muscle without notable visual appearance change. In this study, we used a rapid evaporative ionization mass spectrometry (REIMS) technique for the real-time determination of the extent of repeated freezing and thawing cycles in tuna fillets. We found significant variance in the relative abundance of fatty acids between bluefin tuna and its fresh counterpart following freeze-thaw cycles. Meanwhile, the difference is statistically significant (p < 0.05). The quality of tuna remains largely unaffected by a single freeze-thaw cycle but significantly deteriorates after freeze-thaw cycles (freeze-thaw count ≥2), and the relative fatty acid content of the ionized aerosol analysis in the REIMS system positively correlated with the number of freeze-thaw cycles. Notably, palmitic acid (C 16:0, m/z 255.23), oleic acid (C 18:1, m/z 281.24), and docosahexaenoic acid (C 22:6, m/z 327.23) displayed the most pronounced changes within the spectrum of fatty acid groups.

In this study, an enzymatic reaction was developed for synthesizing pure triacylglycerols (TAG) with a high content of palmitoleic acid (POA) using fish byproduct oil. The characteristics of synthesized structural TAGs rich in POA (POA-TAG) were analyzed in detail through ultrahigh-performance liquid chromatography Q Exactive orbitrap mass spectrometry. Optimal conditions were thoroughly investigated and determined for reaction systems, including the use of Lipozyme TL IM and Novozym 435, 15 wt % lipase loading, substrate mass ratio of 1:3, and water content of 2.5 and 0.5 wt %, respectively, resulting in yields of 67.50 and 67.45% for POA-TAG, respectively. Multivariate statistical analysis revealed that TAG 16:1/16:1/20:4, TAG 16:1/16:1/16:1, TAG 16:1/16:1/18:1, and TAG 16:0/16:1/18:1 were the main variables in Lipozyme TL IM and Novozym 435 enzyme-catalyzed products under different water content conditions. Finally, the fate of POA-TAG across the gastrointestinal tract was simulated using an in vitro digestion model. The results showed that the maximum release of free fatty acids and apparent rate constants were 71.44% and 0.0347 s-1, respectively, for POA-TAG lipids, and the physical and structural characteristics during digestion depended on their microenvironments. These findings provide a theoretical basis for studying the rational design of POA-structural lipids and exploring the nutritional and functional benefits of POA products.

Hypothyroidism has been found to have an effect on the nutritional composition of human milk during pregnancy. This study aims to explore the combined influence of rheological properties, macronutrient content, particle size, and the zeta potential of milk fat globules, as well as the composition of milk fat globule membrane (MFGM) proteins on the quality of human milk in gestational hypothyroidism. The study revealed that human milk from the group with hypothyroidism during pregnancy (AHM) was less viscoelastic and stable when compared with normal pregnancy group human milk (NHM). Furthermore, the particle size and macronutrient content of NHM were found to be larger than that of AHM. In contrast, the zeta potential of AHM was greater than that of NHM. The sodium dodecyl sulfate-PAGE results disclosed that the composition of MFGM proteins in these 2 groups were generally the same, but the content of AHM was lower than that of NHM. In conclusion, this study confirms that hypothyroidism during pregnancy can have a significant effect on the quality of human milk.

In this study, the best solid adsorbent for decolorization was first determined by single-factor test, and then the effects of decolorization temperature, solid adsorbent addition and decolorization time on the decolorization rate of fish oil were investigated. On this basis, the Box-Behnken（BB） experimental design was used to optimize the decolorization conditions of fish oil, and the results of the BB test were analyzed by response surface methodology（RSM） and artificial neural network（ANN）. The results showed that the activated white clay had the best decolorization effect, and the decolorization rate tended to increase and then decrease with the increase of decolorization temperature, solid adsorbent addition and decolorization time; the correlation coefficient r, determination coefficient R~2, root mean square error RMSE and mean square error MSE values of RSM and ANN models were 0.9647, 0.9307, 1.1000, 1.2100 and compared with the RSM model, the ANN model fits better and has less error between the measured and predicted values, so it is more suitable as a prediction model for the decolorization rate of fish oil. Therefore, the RSM and ANN models were selected to jointly optimize the fish oil decolorization process. Firstly, the optimal decolorization conditions were selected by the RSM model, with decolorization temperature of 93.79℃, solid adsorbent addition of 4.80%, and decolorization time of 9.69 min. Subsequently, the above conditions were brought into the ANN model, and the maximum decolorization rate of fish oil was finally obtained as 99.53%. The results of this study showed that the RSM-ANN model has strong accuracy and applicability, which provides a new idea for process optimization in food research.

The illegal adulteration of non-dairy cream in milk fat cream during the manufacturing process of baked goods has significantly hindered the robust growth of the dairy industry. In this study, a method based on rapid evaporative ionization mass spectrometry (REIMS) lipidomics pattern recognition integrated with machine learning algorithms was established. A total of 26 ions with importance were picked using multivariate statistical analysis as salient contributing features to distinguish between milk fat cream and non-dairy cream. Furthermore, employing discriminant analysis, decision trees, support vector machines, and neural network classifiers, machine learning models were utilized to classify non-dairy cream, milk fat cream, and minute quantities of non-dairy cream adulterated in milk fat cream. These approaches were enhanced through hyperparameter optimization and feature engineering, yielding accuracy rates at 98.4-99.6%. This artificial intelligent method of machine learning-guided REIMS pattern recognition can accurately identify adulteration of whipped cream and might help combat food fraud.

Palmitoleic acid (POA) is a monounsaturated n-7 fatty acid (16:1 n-7) that is active in modulating cardiovascular and metabolic processes. POA-structured phospholipids, diglycerides, and triglycerides (POA-PL, -DG, -TG) are abundantly present in marine life. In this study, POA and POA-lipids contained in crude lipids in visceral by-products of six seafood products (n = 6 for each sample) were analyzed using ultra-high-performance liquid chromatography Q-exactive orbitrap mass spectrometry (UHPLC-QE/MS). The results showed that sardine contains the highest percentage of POA (12.47 %), followed by bigeye tuna (7.31 %), whereas silver pomfret contains the lowest percentage (5.76 %) in total lipids. Nine POA-PLs, eight POA-DGs, and 64 POA-TGs were detected, the PCA analysis showed that although the molecular composition six fish species was similar, their relative content varied significantly across the species. The correlation heatmap showed critical POA-PL and POA-DG/TG correlation coefficients and revealed several highly correlated ions. The presence and ratio of POA-PL and POA-DG/TG molecular species led to the identification of each fish species. These findings improve the understanding of the composition of POA-lipids contained in marine by-products and provide a reference for their comprehensive exploitation.

Comprehensive screening for functional substances from natural resources is always a hot research topic. Eicosapentaenoic acid- (EPA) and docosahexaenoic acid (DHA)-structured phospholipids (PLEPA/DHA) have versatile cardiovascular benefits as well as superior bioavailability. Herein, the abundance of PLEPA/DHA in 16 aquatic products was specifically and selectively screened using a recently developed precursor ion scan-driven hydrophilic interaction chromatography-mass spectrometry (PreIS-HILIC/MS) method with the fatty acyl moieties of EPA (m/z 301.6) and DHA (m/z 327.6) locked. The aim focused on the characteristics and differences in the varieties and contents of EPA/DHA-structured phosphatidylcholine (PCEPA/DHA) and EPA/DHA-structured phosphatidylethanolamine (PEEPA/DHA) molecular species. A total of 80 PLEPA/DHA molecules were identified in these natural sources, including 47 PCEPA/DHA and 33 PEEPA/DHA. After analysis, PC 16:0/20:5 and PC 16:0/22:6 are present in all aquatic products and at high levels. Antarctic krill was found to be the best resource of PLEPA/DHA in total (2574.69 μg·g-1), followed by mackerel (2330.11 μg·g-1), salmon (2109.91 μg·g-1), and Farrer's scallop (1883.59 μg·g-1), while abalone contained the lowest level of PLEPA/DHA (310.44 μg·g-1). Besides, sea cucumber and sea bass contained the highest contents of EPA-structured and DHA-structured ether phospholipids, respectively, which could be highly recommended as dietary sources of special functional phospholipids. Finally, the multiple discrepancies between the 16 aquatic products were revealed by multivariate statistical analysis. These findings improve the awareness of the composition and content of PLEPA/DHA contained in aquatic products, providing a reference for their integrated development.

采用脱胶、脱酸、脱色、脱臭工艺精制金枪鱼油,探究低温结晶法对精制鱼油中甘油三酯型二十碳五烯酸(EPA)和二十二碳六烯酸(DHA)的富集效果.结果表明:精制鱼油各项指标均达到一级质量标准.其饱和脂肪酸含量下降,单不饱和脂肪酸和多不饱和脂肪酸含量有所上升,EPA和DHA含量分别为6.69％和16.46％;甘油三酯的含量为97.62％.低温结晶法最佳富集条件是:溶剂为乙腈与丙酮,结晶温度-50℃,乙腈与丙酮复配比1:12(V/V),鱼油与复合溶剂(乙腈与丙酮)比7:40(V/V),结晶时间150 min.在此条件下,多不饱和脂肪酸含量达51.61％,其中EPA与DHA含量分别为(12.83±0.34)％和(28.70±0.48)％,得率分别为(40.10±1.07)％和(36.52±2.53)％.

The fish fillets of basa catfish (Pangasius bocourti) and sole fish (Cynoglossus semilaevis Gunther) have similar appearance but different market values, leading to the possibility of adulteration for economic gains. In this study, a surgical knife, namely iKnife, was coupled to rapid evaporative ionization mass spectrometry (REIMS) to develop a high-throughput technique for in situ and real-time authenticating these two fish species. The iKnife generated informative aerosol, which was further aspired into mass spectrometry to acquire specific fingerprinting profiles. The spectra were multivariate statistical analyzed, and the most contributing ions responsible for the significant difference between the lipidomics profiles of basa catfish and sole fish were screened out. For instance, ions of m/z 281.2470, 279.2319, 699.4970, etc. were abundance in basa catfish, while m/z 301.2164, 327.2341, 764.5284, etc. were significant in sole fish. Subsequently, the validation of the method was carried out in terms of intra-day precision (RSD 5.06%–8.65%) and inter-day precision (RSD ≤9.17%). Finally, this established iKnife-REIMS method was successfully applied to blind samples from markets with an accuracy greater than 98%. The results indicated that the proposed iKnife REIMS method could be used to unambiguously authenticate these two easily adulterated basa catfish and sole fish, and provide the basis and potential for the high-throughput identification of marine resources on the market.

海洋生物体内含有丰富的ω-3多不饱和脂肪酸(PUFAs),特别是二十碳五烯酸(EPA)和二十二碳六烯酸(DHA),在预防心血管疾病,抑制癌症、抗炎,促进大脑发育等方面发挥重要作用,故而在保健品、医药行业潜力巨大.本文首先简述ω-3 PUFAs的膳食结构及其在海洋中不同的生物来源,其次详细对比不同结构的ω-3 PUFAs体内代谢差异,最后总结ω-3 PUFAs分离纯化方法,以期为ω-3 PUFAs在功能食品、医药领域的进一步探索与开发提供理论参考.

The price of mammalian milk from different animal species varies greatly due to differences in their yield and nutritional value. Therefore, the authenticity of dairy products has become a hotspot issue in the market due to the replacement or partial admixture of high-cost milk with its low-cost analog. Herein, four common commercial varieties of milk, including goat milk, buffalo milk, Holstein cow milk, and Jersey cow milk, were successfully profiled and differentiated from each other by rapid evaporative ionization mass spectrometry (REIMS) combined with chemometric analysis. This method was developed as a real-time lipid fingerprinting technique. Moreover, the established chemometric algorithms based on multivariate statistical methods mainly involved principal component analysis, orthogonal partial least squares-discriminant analysis, and linear discriminant analysis as the screening and verifying tools to provide insights into the distinctive molecules constituting the four varieties of milk. The ions with m/z 229.1800, 243.1976, 257.2112, 285.2443, 299.2596, 313.2746, 341.3057, 355.2863, 383.3174, 411.3488, 439.3822, 551.5051, 577.5200, 628.5547, 656.5884, 661.5455, 682.6015, and 684.6146 were selected as potential classified markers. The results of the present work suggest that the proposed method could serve as a reference for recognizing dairy fraudulence related to animal species and expand the application field of REIMS technology.

Trichiurus lepturus (hairtail) is an important economic component of China’s marine fishing industry. However, due to the difficulty in identifying the appearance of hairtail from different geographical distributions, hairtails with geographical indication trademarks were imitated by general varieties. In this study, the texture characteristics, color, basic nutrients, amino acids, mineral, fatty acids, and volatile flavor substances were used as indicators for multivariate statistical analysis to determine whether three origins of hairtails from the habitats of Zhoushan (East China Sea, T.Z), Hainan (South China Sea, T.N), and Qingdao (Yellow Sea, T.Q) in the market could be distinguished. The findings revealed that there were significant differences in amino acids composition, mineral composition, fatty acid composition in lipids, and volatile flavor substances among the hairtails of three origins (P < 0.05), but no differences in color, texture, protein content. T.Z had moisture, crude fat, essential amino acids (EAA), flavor amino acids (FAA), unsaturated fatty acids (UFA), and docosahexaenoic acids and dicosapentaenoic acids (ΣEPA + DHA) contents of 74.33, 5.4%, 58.25 mg⋅g–1, 46.20 mg⋅g–1, 66.84 and 19.38%, respectively, and the contents of volatile alcohols, aldehydes and ketones were 7.44, 5.30, and 5.38%, respectively. T.N contains moisture, crude fat, EAA, FAA, UFA and ΣEPA + DHA as 77.69, 2.38%, 64.76 mg⋅g–1, 52.44 mg⋅g–1, 65.52 and 29.45%, respectively, and the contents of volatile alcohols, aldehydes and ketones as 3.21, 8.92, and 10.98%, respectively. T.Q had the contents of moisture, crude fat, EAA, FAA, UFA, and ΣEPA + DHA 79.69, 1.43%, 60.9 mg⋅g–1, and 49.42 mg⋅g–1, respectively. The contents of unsaturated fatty acid and ΣEPA + DHA were 63.75 and 26.12%, respectively, while the volatile alcohols, aldehydes, and ketones were 5.14, 5.99, and 7.85%, respectively. Partial least squares-discriminant analysis (PLS-DA) multivariate statistical analysis showed that volatile flavor compounds could be used as the most ideal indicators for tracing the source of hairtail. In conclusion, the findings of this study can distinguish the three hairtail origins using some basic indicators, providing ideas for hairtail geographical identification.

As a high-value processed aquatic product, wet-aged tuna has gradually become a popular food, but its lipidomics characteristics during the aging process have not been investigated. Herein, the lipidomics phenotypic data of tuna at different wet-aging stages were acquired using iKnife rapid evaporative ionization mass spectrometry, in which the dominant lipid components, including fatty acid (FA), phosphatidylcholine (PC), phosphatidylethanolamine (PE), and phosphatidylinositol (PI), were structurally identified. Principal component analysis, permutation test, heatmap, and circos plot analysis were performed to characterize lipids in wet-aged tuna, among which FAC18:1, docosahexaenoic acid (DHA), and PIC18:0/22:6 were the most contributing components for determining the wet-aging stage of tuna. The results indicated that iKnife-REIMS is accurate (86.5%), reliable, and could be used in the real-time detection of tuna meat during different wet-aging stages.

Minced shrimp is popular seafood due to its delicious flavor and nutritional value. However, the biological species of raw material of minced shrimp are not distinguished by naked eyes after processing. Thus, an in situ and real-time minced shrimp authentication method was established using iKnife rapid evaporative ionization mass spectrometry (REIMS) based lipidomics. The samples were analyzed under ambient ionization without any tedious preparation step. Seven economic shrimp samples were tested, whose phenotypes were used to develop a real-time recognition model. A total of 19 fatty acids and 45 phospholipid molecular species were efficiently identified and statistically analyzed by multivariate statistical analysis. The results showed that the seven shrimp species were well distinguished, and the most contributing ions at m/z 255.2, 279.2, 301.2, 327.2, 699.5, 742.5, etc., were revealed by variable importance in projection. The proposed iKnife REIMS showed excellent performance in minced shrimp authentication.