Untargeted lipidomics using liquid chromatography-ion mobility-mass spectrometry reveals novel triacylglycerides in human milk

George, Alexandra D.; Gay, Melvin; Wlodek, Mary E.; Trengove, Robert D.; Murray, Kevin; Geddes, Donna T.

doi:10.1038/s41598-020-66235-y

Cited by 32 publications

(19 citation statements)

References 56 publications

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“…However, for the use of IM-MS data for compound identification, the compilation of comprehensive databases containing CCS values of the compounds of interest is essential. In the past, the focus of available databases was on endogenous compounds, such as peptides, glycans, lipids, and steroids, reflecting that omics-based studies in different fields, such as metabolomics, , lipidomics, , plantomics, or proteomics, have been the predominant recent application of IM-MS. Yet, interest in the use of IM-MS for the analysis of CECs is rising.…”

Section: Introductionmentioning

confidence: 99%

Ion Mobility-High-Resolution Mass Spectrometry (IM-HRMS) for the Analysis of Contaminants of Emerging Concern (CECs): Database Compilation and Application to Urine Samples

2021

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Ion mobility mass spectrometry (IM-MS)-derived collision cross section (CCS) values can serve as a valuable additional identification parameter within the analysis of compounds of emerging concern (CEC) in human matrices. This study introduces the first comprehensive database of DTCCSN2 values of 148 CECs and their metabolites including bisphenols, alternative plasticizers (AP), organophosphate flame retardants (OP), perfluoroalkyl chemicals (PFAS), and others. A total of 311 ions were included in the database, whereby the DTCCSN2 values for 113 compounds are reported for the first time. For 105 compounds, more than one ion is reported. Moreover, the DTCCSN2 values of several isomeric CECs and their metabolites are reported to allow a distinction between isomers. Comprehensive quality assurance guidelines were implemented in the workflow of acquiring DTCCSN2 values to ensure reproducible experimental conditions. The reliability and reproducibility of the complied database were investigated by analyzing pooled human urine spiked with 30 AP and OP metabolites at two concentration levels. For all investigated metabolites, the DTCCSN2 values measured in urine showed a percent error of <1% in comparison to database values. DTCCSN2 values of OP metabolites showed an average percent error of 0.12% (50 ng/mL in urine) and 0.15% (20 ng/mL in urine). For AP metabolites, these values were 0.10 and 0.09%, respectively. These results show that the provided database can be of great value for enhanced identification of CECs in environmental and human matrices, which can advance future suspect screening studies on CECs.

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Section: Introductionmentioning

confidence: 99%

Ion Mobility-High-Resolution Mass Spectrometry (IM-HRMS) for the Analysis of Contaminants of Emerging Concern (CECs): Database Compilation and Application to Urine Samples

2021

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“…For example, lipids are most often regarded as nutrition but there is mounting evidence of their association with health. Using new methods [ 258 ] we have recently discovered 98 novel triaclyerglicerides (TAGs) and found that infant intake of palmitic acid-containing and lauric acid-containing TAGs differed between healthy and unwell infants indicating responsiveness of the milk [ 259 ]. This is consistent with our previous study that showed reductions in the proportion of capric (C10:0) and lauric acids and increases in palmitoleic and stearic acid [ 260 ] in unwell mothers and infants.…”

Section: Infant Healthmentioning

confidence: 99%

25 Years of Research in Human Lactation: From Discovery to Translation

et al. 2021

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Researchers have recently called for human lactation research to be conceptualized as a biological framework where maternal and infant factors impacting human milk, in terms of composition, volume and energy content are studied along with relationships to infant growth, development and health. This approach allows for the development of evidence-based interventions that are more likely to support breastfeeding and lactation in pursuit of global breastfeeding goals. Here we summarize the seminal findings of our research programme using a biological systems approach traversing breast anatomy, milk secretion, physiology of milk removal with respect to breastfeeding and expression, milk composition and infant intake, and infant gastric emptying, culminating in the exploration of relationships with infant growth, development of body composition, and health. This approach has allowed the translation of the findings with respect to education, and clinical practice. It also sets a foundation for improved study design for future investigations in human lactation.

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“…Additionally, methodologies encompassing shot-gun or direct infusion versus separation by liquid chromatography before MS detection are currently used and are a matter of debate regarding their efficiency [ 5 , 6 , 16 ]. Therefore, active research concerning the influence of other factors on the fragmentation information quality, as well as the application of diverse methodologies, is ongoing at present regarding TAG analysis [ 17 , 18 , 19 , 20 , 21 , 22 , 23 , 24 , 25 ].…”

Section: Introductionmentioning

confidence: 99%

Ammonia Concentration in the Eluent Influences Fragmentation Pattern of Triacylglycerols in Mass Spectrometry Analysis

2022

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Correct assessment of the fatty acyl at the glycerol sn-2 position in triacylglycerol (TAG) analysis by liquid chromatography and mass spectrometry (LC-MS) is challenging. Ammonium hydroxide (NH4OH) is the preferred choice for the solvent additive for the formation of the ammonium adduct ([M + NH4]+). In this study, the influence of different NH4OH concentrations in the eluents on TAG adduct formation and fragmentation under LC-MS analysis was assessed. Increasing NH4OH concentrations delayed the chromatographic elution time according to a power function. The [M + NH4]+ and [M + ACN + NH4]+ adducts (where ACN means acetonitrile) were formed at all ammonium concentrations assayed. [M + ACN + NH4]+ predominated above 18.26 mM [NH4OH], and the intensity of [M + NH4]+ dropped. TAG fragmentation for fatty acyl release in the MSE was reduced with increasing [M + ACN + NH4]+ adduct, which suggests that ACN stabilizes the adduct in a way that inhibits the rupture of the ester bonds in TAGs. A linear equation (Hsn-I = a × H[M+NH4]+, where sn-I refers to the sn position of the glycerol (I = 1, 2, or 3) and H is the peak height) was deduced to quantify the dehydroxydiacylglycerol fragment intensity in relation to [M + NH4]+ intensity in the full scan. This equation had a slope mean value of 0.369 ± 0.058 for the sn-1 and sn-3 positions, and of 0.188 ± 0.007 for the sn-2 position.

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Untargeted lipidomics using liquid chromatography-ion mobility-mass spectrometry reveals novel triacylglycerides in human milk

Cited by 32 publications

References 56 publications

Ion Mobility-High-Resolution Mass Spectrometry (IM-HRMS) for the Analysis of Contaminants of Emerging Concern (CECs): Database Compilation and Application to Urine Samples

Ion Mobility-High-Resolution Mass Spectrometry (IM-HRMS) for the Analysis of Contaminants of Emerging Concern (CECs): Database Compilation and Application to Urine Samples

25 Years of Research in Human Lactation: From Discovery to Translation

Ammonia Concentration in the Eluent Influences Fragmentation Pattern of Triacylglycerols in Mass Spectrometry Analysis

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