{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,8,5]],"date-time":"2026-08-05T15:09:22Z","timestamp":1785942562291,"version":"3.56.0"},"reference-count":47,"publisher":"American Chemical Society (ACS)","issue":"30","license":[{"start":{"date-parts":[[2026,7,25]],"date-time":"2026-07-25T00:00:00Z","timestamp":1784937600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,7,25]],"date-time":"2026-07-25T00:00:00Z","timestamp":1784937600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,7,25]],"date-time":"2026-07-25T00:00:00Z","timestamp":1784937600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/501100002241","name":"Japan Science and Technology Agency","doi-asserted-by":"publisher","award":["JPMJPF2108"],"award-info":[{"award-number":["JPMJPF2108"]}],"id":[{"id":"10.13039\/501100002241","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100025019","name":"Support for Pioneering Research Initiated by the Next Generation","doi-asserted-by":"publisher","award":["JPMJSP2119"],"award-info":[{"award-number":["JPMJSP2119"]}],"id":[{"id":"10.13039\/501100025019","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,5]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Human milk oligosaccharides (HMOs) are bioactive components of human breast milk (HBM), but their concentrations vary with maternal secretor phenotype and lactation stage, making individual HMO quantification analytically demanding. Here, we present a reference-guided benchtop 60 MHz NMR workflow integrating chemometrics and machine learning to quantify major fucosylated HMOs in HBM. A total of 111 HBM samples from 37 donors across lactation stages were analyzed. Using 800 MHz NMR-derived concentrations as references, predictive models were developed from benchtop NMR spectra for 2\u2032-fucosyllactose (2\u2032-FL), 3-fucosyllactose (3-FL), and lacto-N-fucopentaose I (LNFP-I). Unlike conventional peak-fitting-based NMR quantification, this workflow recovered HMO-specific quantitative information from highly overlapped 60 MHz carbohydrate signals that were not directly resolvable in authentic HBM. Elastic Net yielded practical models, particularly for lower-abundance 3-FL and LNFP-I. These results support benchtop NMR combined with machine learning as an accessible platform for HMO screening.<\/jats:p>","DOI":"10.1021\/acs.jafc.6c04775","type":"journal-article","created":{"date-parts":[[2026,7,27]],"date-time":"2026-07-27T05:11:30Z","timestamp":1785129090000},"page":"23924-23934","source":"Crossref","is-referenced-by-count":0,"title":["Machine Learning-Enabled\nQuantification of Fucosylated\nHuman Milk Oligosaccharides in Human Breast Milk by Benchtop 1H NMR Spectroscopy"],"prefix":"10.1021","volume":"74","author":[{"given":"Zhiyan","family":"Hu","sequence":"first","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiaxi","family":"Jiang","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun","family":"Abe","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Thanawat","family":"Thumrongtaradol","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-2887-2360","authenticated-orcid":true,"given":"Miho","family":"Akasaka","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuki","family":"Ohnishi","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Seiji","family":"Osada","sequence":"additional","affiliation":[{"name":"Ltd. , , Hitachi , ,","place":["Ibaraki, Japan, 317-0075"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2328-9519","authenticated-orcid":true,"given":"Tatsuya","family":"Arai","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3713-2122","authenticated-orcid":true,"given":"Hiroyuki","family":"Kumeta","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yasuhiro","family":"Kumaki","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kazuo","family":"Yamauchi","sequence":"additional","affiliation":[{"name":"Niigata University , , , ,","place":["Niigata, Niigata, Japan, 950-2181"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu","family":"Shimizu","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 001-0021"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuki","family":"Yokoi","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 001-0021"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kiminori","family":"Nakamura","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 001-0021"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tokiyoshi","family":"Ayabe","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 001-0021"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Koshi","family":"Nakamura","sequence":"additional","affiliation":[{"name":"University of the Ryukyus , , , ,","place":["Ginowan, Okinawa, Japan, 910-2770"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Takashi","family":"Kimura","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-8638"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Akiko","family":"Tamakoshi","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-8638"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9134-7576","authenticated-orcid":true,"given":"Tomoyasu","family":"Aizawa","sequence":"additional","affiliation":[{"name":"Hokkaido University , , , ,","place":["Sapporo, Hokkaido, Japan, 060-0810"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,25]]},"reference":[{"issue":"2","key":"2026080510083182300_cit1","doi-asserted-by":"publisher","first-page":"278S","DOI":"10.3945\/ajcn.2010.29459","article-title":"Overview of Nutrients in Human Milk","volume":"9","author":"Fischer","year":"2018","journal-title":"Adv. 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Dev."},{"issue":"8","key":"2026080510083182300_cit4","doi-asserted-by":"publisher","first-page":"2737","DOI":"10.3390\/nu13082737","article-title":"The Mean of Milk: A Review of Human\nMilk Oligosaccharide Concentrations throughout Lactation","volume":"13","author":"Soyy\u0131lmaz","year":"2021","journal-title":"Nutrients"},{"issue":"9","key":"2026080510083182300_cit5","doi-asserted-by":"publisher","first-page":"1147","DOI":"10.1093\/glycob\/cws074","article-title":"Human Milk\nOligosaccharides: Every Baby Needs a Sugar Mama","volume":"22","author":"Bode","year":"2012","journal-title":"Glycobiology"},{"issue":"10","key":"2026080510083182300_cit6","doi-asserted-by":"publisher","first-page":"5563","DOI":"10.1021\/acs.analchem.4c06081","article-title":"Robust and High-Resolution All-Ion Fragmentation LC-ESI-IM-MS Analysis\nfor In-Depth Characterization or Profiling of Up to 200 Human Milk\nOligosaccharides","volume":"97","author":"Gonsalves","year":"2025","journal-title":"Anal. Chem."},{"issue":"1","key":"2026080510083182300_cit7","doi-asserted-by":"publisher","first-page":"2186115","DOI":"10.1080\/19490976.2023.2186115","article-title":"Functional\nEffects of Human Milk Oligosaccharides (HMOs)","volume":"15","author":"Dinleyici","year":"2023","journal-title":"Gut Microbes"},{"issue":"1","key":"2026080510083182300_cit8","doi-asserted-by":"publisher","first-page":"108","DOI":"10.1186\/s12934-021-01599-y","article-title":"Gold Standard\nfor Nutrition: A Review of Human Milk Oligosaccharide\nand Its Effects on Infant Gut Microbiota","volume":"20","author":"Zhang","year":"2021","journal-title":"Microb.\nCell Fact."},{"key":"2026080510083182300_cit9","doi-asserted-by":"publisher","first-page":"1523829","DOI":"10.3389\/fimmu.2024.1523829","article-title":"Interactions\nof Human Milk Oligosaccharides\nwith the Immune System","volume":"15","author":"Slater","year":"2025","journal-title":"Front. Immunol."},{"issue":"9","key":"2026080510083182300_cit10","doi-asserted-by":"publisher","first-page":"4640","DOI":"10.1074\/jbc.270.9.4640","article-title":"Sequence\nand Expression of a Candidate for the Human Secretor Blood Group \u03b1(1,2)Fucosyltransferase\nGene (FUT2): HOMOZYGOSITY FOR AN ENZYME-INACTIVATING NONSENSE MUTATION\nCOMMONLY CORRELATES WITH THE NON-SECRETOR PHENOTYPE","volume":"270","author":"Kelly","year":"1995","journal-title":"J. Biol. Chem."},{"key":"2026080510083182300_cit11","doi-asserted-by":"publisher","first-page":"4193","DOI":"10.1073\/pnas.81.13.4193","article-title":"Biochemical Evidence That Secretor Gene, Se, Is a Structural\nGene Encoding a Specific Fucosyltransferase","volume":"81","author":"Kumazaki","year":"1984","journal-title":"Med. Sci."},{"key":"2026080510083182300_cit12","doi-asserted-by":"publisher","first-page":"103058","DOI":"10.1016\/j.cdnut.2024.103058","article-title":"Maternal FUT2\nSecretor Phenotype\nIs Associated With Human Milk Oligosaccharides and Polyphenol Metabolites\nFollowing a Mediterranean Dietary Intervention: A Pilot Study","volume":"8","author":"Fiecke","year":"2024","journal-title":"Curr. Dev. Nutr."},{"issue":"6","key":"2026080510083182300_cit13","doi-asserted-by":"publisher","first-page":"1408","DOI":"10.3390\/nu15061408","article-title":"Human Milk\nOligosaccharides Are Associated with Lactation Stage and Lewis Phenotype\nin a Chinese Population","volume":"15","author":"Ren","year":"2023","journal-title":"Nutrients"},{"issue":"42","key":"2026080510083182300_cit14","doi-asserted-by":"publisher","first-page":"15553","DOI":"10.1021\/acs.jafc.3c03181","article-title":"Qualitative\nand Quantitative Changes of Oligosaccharides in Human and Animal Milk\nover Lactation","volume":"71","author":"Zhang","year":"2023","journal-title":"J. Agric. Food Chem."},{"issue":"51","key":"2026080510083182300_cit15","doi-asserted-by":"publisher","first-page":"15585","DOI":"10.1021\/acs.jafc.1c05872","article-title":"Comprehensive Identification and\nAbsolute Quantification of Milk Oligosaccharides in Different Species","volume":"69","author":"Shi","year":"2021","journal-title":"J. Agric. Food Chem."},{"issue":"6","key":"2026080510083182300_cit16","doi-asserted-by":"publisher","first-page":"328","DOI":"10.1016\/j.carbpol.2019.04.092","article-title":"Absolute Quantification\nof Twelve Oligosaccharides in Human Milk Using a Targeted Mass Spectrometry-Based\nApproach","volume":"219","author":"Zhang","year":"2019","journal-title":"Carbohydr. Polym."},{"key":"2026080510083182300_cit17","doi-asserted-by":"publisher","first-page":"142821","DOI":"10.1016\/j.foodchem.2025.142821","article-title":"Quantitative Nuclear Magnetic Analysis\nof Human Milk Oligosaccharides 2\u2019-Fucosyllactose and 3-Fucosyllactose\nin Complicated Food Matrices","volume":"473","author":"An","year":"2025","journal-title":"Food Chem."},{"key":"2026080510083182300_cit18","doi-asserted-by":"publisher","first-page":"813690","DOI":"10.3389\/fnut.2021.813690","article-title":"Dynamic Associations\nof Milk Components With the Infant Gut Microbiome and Fecal Metabolites\nin a Mother\u2013Infant Model by Microbiome, NMR Metabolomic, and\nTime-Series Clustering Analyses","volume":"8","author":"Komatsu","year":"2022","journal-title":"Front. Nutr."},{"issue":"19","key":"2026080510083182300_cit19","doi-asserted-by":"publisher","first-page":"9887","DOI":"10.1021\/ac5025039","article-title":"Precision\nHigh-Throughput Proton NMR Spectroscopy of\nHuman Urine, Serum, and Plasma for Large-Scale Metabolic Phenotyping","volume":"86","author":"Dona","year":"2014","journal-title":"Anal. Chem."},{"issue":"1","key":"2026080510083182300_cit20","doi-asserted-by":"publisher","first-page":"290","DOI":"10.3168\/jds.2012-5819","article-title":"Nuclear Magnetic\nResonance Metabonomics Reveals Strong Association between Milk Metabolites\nand Somatic Cell Count in Bovine Milk","volume":"96","author":"Sundekilde","year":"2013","journal-title":"J. Dairy\nSci."},{"key":"2026080510083182300_cit21","doi-asserted-by":"publisher","first-page":"5","DOI":"10.1016\/j.trac.2012.02.007","article-title":"Quantitative 1H NMR\nSpectroscopy","volume":"35","author":"Bharti","year":"2012","journal-title":"TrAC, Trends\nAnal. 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Anal."},{"issue":"5","key":"2026080510083182300_cit24","doi-asserted-by":"publisher","first-page":"611","DOI":"10.3390\/metabo13050611","article-title":"Application of Benchtop\nNMR for Metabolomics Study Using Feces of Mice with DSS-Induced Colitis","volume":"13","author":"Song","year":"2023","journal-title":"Metabolites"},{"issue":"2","key":"2026080510083182300_cit25","doi-asserted-by":"publisher","DOI":"10.1002\/nbm.70215","article-title":"Detection\nLimits of Blood Metabolites at Physiological Concentrations Using\nBenchtop 1$$ {}\u03021 $$H NMR","volume":"39","author":"Hill","year":"2026","journal-title":"NMR Biomed."},{"key":"2026080510083182300_cit26","doi-asserted-by":"publisher","first-page":"118371","DOI":"10.1016\/j.microc.2026.118371","article-title":"Benchtop NMR-Based Lactose Quantification in Human\nMilk: Correction of Oligosaccharide Interference and Comparison with\nHigh-Field NMR","volume":"226","author":"Jiang","year":"2026","journal-title":"Microchem. 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Biomol. Spectrosc."},{"issue":"12","key":"2026080510083182300_cit30","doi-asserted-by":"publisher","first-page":"6399","DOI":"10.1021\/acs.analchem.4c04660","article-title":"Benchtop\nProton NMR Spectroscopy for High-Throughput Lipoprotein Quantification\nin Human Serum and Plasma","volume":"97","author":"Wist","year":"2025","journal-title":"Anal. Chem."},{"key":"2026080510083182300_cit31","doi-asserted-by":"publisher","first-page":"111034","DOI":"10.1016\/j.foodhyd.2024.111034","article-title":"Inter-Individual\nVariation in Human Microbiota Drives Differential Impacts on the Fermentability\nof Insoluble Bran by Soluble \u03b2-Glucans from Whole Barley","volume":"162","author":"Fan","year":"2025","journal-title":"Food Hydrocoll"},{"issue":"47","key":"2026080510083182300_cit32","doi-asserted-by":"publisher","first-page":"29998","DOI":"10.1021\/acs.jafc.5c08522","article-title":"Recent Advances\nin Integrating Machine Learning with Omics Approaches in Food Science\nand Nutrition Research","volume":"73","author":"Xiao","year":"2025","journal-title":"J. Agric. Food Chem."},{"key":"2026080510083182300_cit33","doi-asserted-by":"publisher","first-page":"146008","DOI":"10.1016\/j.foodchem.2025.146008","article-title":"Classification\nand Quantification of Sesame Oil in Edible Oils and\nAdulterated Mixtures Using 1H NMR Spectroscopy Combined with Multivariate,\nMachine Learning, and Deep Learning Models","volume":"493","author":"Lim","year":"2025","journal-title":"Food Chem."},{"key":"2026080510083182300_cit34","doi-asserted-by":"publisher","first-page":"147","DOI":"10.1016\/j.trac.2014.02.006","article-title":"60 MHz 1H NMR Spectroscopy\nfor the Analysis of Edible\nOils","volume":"57","author":"Parker","year":"2014","journal-title":"TrAC, Trends Anal. Chem."},{"issue":"2","key":"2026080510083182300_cit35","doi-asserted-by":"publisher","first-page":"301","DOI":"10.1111\/j.1467-9868.2005.00503.x","article-title":"Regularization and Variable Selection Via the Elastic\nNet","volume":"67","author":"Zou","year":"2005","journal-title":"J. R. Stat. Soc. Series B Stat. Methodol."},{"key":"2026080510083182300_cit36","doi-asserted-by":"publisher","first-page":"110753","DOI":"10.1016\/j.foodcont.2024.110753","article-title":"Machine Learning-Enabled Fatty Acid\nQuantification\nand Classification of Pork from Autochthonous Breeds Using Low-Field\n1H NMR Spectroscopic Data","volume":"166","author":"Ramiro","year":"2024","journal-title":"Food Control"},{"key":"2026080510083182300_cit37","doi-asserted-by":"publisher","first-page":"5","DOI":"10.1023\/A:1010933404324","article-title":"Random Forests","volume":"45","author":"Breiman","year":"2001"},{"issue":"1","key":"2026080510083182300_cit38","doi-asserted-by":"publisher","first-page":"213","DOI":"10.1186\/1471-2105-10-213","article-title":"A Comparison\nof Random Forest and Its Gini Importance with Standard Chemometric\nMethods for the Feature Selection and Classification of Spectral Data","volume":"10","author":"Menze","year":"2009","journal-title":"BMC Bioinf."},{"issue":"9","key":"2026080510083182300_cit39","doi-asserted-by":"publisher","first-page":"1073","DOI":"10.1016\/j.trac.2010.05.006","article-title":"Critical Review\nof Chemometric Indicators Commonly Used for Assessing the Quality\nof the Prediction of Soil Attributes by NIR Spectroscopy","volume":"29","author":"Bellon-Maurel","year":"2010","journal-title":"TrAC, Trends Anal. Chem."},{"issue":"6","key":"2026080510083182300_cit40","doi-asserted-by":"publisher","first-page":"3279","DOI":"10.1021\/jf100420z","article-title":"Use of Attenuated\nTotal Reflectance Midinfrared for Rapid and Real-Time Analysis of\nCompositional Parameters in Commercial White Grape Juice","volume":"58","author":"Shah","year":"2010","journal-title":"J. Agric. Food Chem."},{"issue":"3","key":"2026080510083182300_cit41","doi-asserted-by":"publisher","first-page":"211","DOI":"10.1002\/cem.1180020306","article-title":"PLS Regression\nMethods","volume":"2","author":"Ho\u0308skuldsson","year":"1988","journal-title":"J. Chemom."},{"issue":"2","key":"2026080510083182300_cit42","doi-asserted-by":"publisher","first-page":"109","DOI":"10.1016\/S0169-7439(01)00155-1","article-title":"PLS-Regression:\nA Basic\nTool of Chemometrics","volume":"58","author":"Wold","year":"2001","journal-title":"Chemom. Intell. Lab. Syst."},{"issue":"7","key":"2026080510083182300_cit43","doi-asserted-by":"publisher","first-page":"110095","DOI":"10.1016\/j.microc.2024.110095","article-title":"A New Application of\nElasticnet Regression Based Near-Infrared\nSpectroscopy Model: Prediction and Analysis of 2,3,5,4\u2032-Tetrahydroxy\nStilbene-2-O-\u03b2-D-Glucoside and Moisture in Polygonum Multiflorum","volume":"199","author":"Liu","year":"2024","journal-title":"Microchem. 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