{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,22]],"date-time":"2026-09-22T16:11:55Z","timestamp":1790093515721,"version":"4.0.1"},"reference-count":51,"publisher":"American Chemical Society (ACS)","issue":"37","license":[{"start":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T00:00:00Z","timestamp":1788739200000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by-nc-nd\/4.0\/"}],"funder":[{"DOI":"10.13039\/100011660","name":"Idaho National Laboratory","doi-asserted-by":"publisher","award":["DE-AC07-05ID14517"],"award-info":[{"award-number":["DE-AC07-05ID14517"]}],"id":[{"id":"10.13039\/100011660","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100005825","name":"National Institute of Food and Agriculture","doi-asserted-by":"publisher","award":["2024-69012-41754"],"award-info":[{"award-number":["2024-69012-41754"]}],"id":[{"id":"10.13039\/100005825","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100005825","name":"National Institute of Food and Agriculture","doi-asserted-by":"publisher","award":["2025-69016-44434"],"award-info":[{"award-number":["2025-69016-44434"]}],"id":[{"id":"10.13039\/100005825","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,9,22]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>The valorization of technical lignin requires fractionation strategies that deliver chemically and thermally distinct lignin streams with predictable structure\u2013property relationships while minimizing hazardous solvent use. Here, we propose a preliminary, exploratory thermodynamic design framework for lignin fractionation based on deep eutectic solvents (DESs), using activity coefficients as quantitative descriptors of solvent\u2013solute interactions. Six chloride-based DESs were synthesized and characterized through freezing-point depression, FTIR spectroscopy, and Schro\u0308der\u2013Le Chatelier analysis. All eutectic compositions exhibited negative deviations from ideality (\u03b3 &amp;lt; 1), consistent with strong hydrogen-bond interactions. Importantly, lignin solubility and solvent stability were highest among the systems studied within an apparent, exploratory activity-coefficient window (0.2 &amp;lt; \u03b3 &amp;lt; 1), supporting rational DES pre-screening that should be validated across a broader range of DES chemistries without extensive empirical screening. Guided by these heuristics, two optimized, sulfur-free DESs (ChCl\/levulinic acid and tetrabutylammonium chloride\/ethylene glycol) were applied in sequential fractionation of industrial softwood kraft lignin, yielding four distinct fractions. Structural and elemental analyses suggested reduced apparent molecular weight, lower methoxyl content, and increased hydrogen content, while thermal analysis showed substantially decreased glass transition temperatures (&amp;lt;100 \u00b0C). These results suggest that activity-coefficient-guided DES selection offers a promising strategy for upgrading heterogeneous kraft lignin into thermally compatible fractions, representing an early step toward predictive solvent engineering for lignin valorization.<\/jats:p>","DOI":"10.1021\/acsomega.6c02769","type":"journal-article","created":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T06:01:34Z","timestamp":1788760894000},"page":"55184-55196","source":"Crossref","is-referenced-by-count":0,"title":["Activity-Coefficient-Guided\nHeuristics for Deep Eutectic\nSolvent Fractionation of Kraft Lignin"],"prefix":"10.1021","volume":"11","author":[{"given":"Gloria","family":"Agyapong","sequence":"first","affiliation":[{"name":"University of Maine , , , ,","place":["Orono, Maine, United States, 04469"]},{"name":"University of Maine , , , ,","place":["Orono, Maine, United States, 04469"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5376-3330","authenticated-orcid":true,"given":"Regan","family":"Ceaser","sequence":"additional","affiliation":[{"name":"University of Maine , , , ,","place":["Orono, Maine, United States, 04469"]},{"name":"University of Maine , , , ,","place":["Orono, Maine, United States, 04469"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1935-0110","authenticated-orcid":true,"given":"C. Luke","family":"Williams","sequence":"additional","affiliation":[{"name":"Idaho National Laboratory , , , ,","place":["Idaho Falls, Idaho, United States, 83415"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1113-1324","authenticated-orcid":true,"given":"M.Clayton","family":"Wheeler","sequence":"additional","affiliation":[{"name":"University of Maine , , , ,","place":["Orono, Maine, United States, 04469"]},{"name":"University of Maine , , , ,","place":["Orono, Maine, United States, 04469"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7297-3993","authenticated-orcid":true,"given":"Sampath","family":"Gunukula","sequence":"additional","affiliation":[{"name":"University of Maine , , , ,","place":["Orono, Maine, United States, 04469"]},{"name":"University of Maine , , , ,","place":["Orono, Maine, United States, 04469"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,7]]},"reference":[{"issue":"50","key":"2026092210580951900_cit1","doi-asserted-by":"publisher","first-page":"18577","DOI":"10.1021\/acssuschemeng.0c06655","article-title":"Kraft Lignin Solubility and Its Chemical Modification\nin Deep Eutectic Solvents","volume":"8","author":"Sosa","year":"2020","journal-title":"ACS Sustainable Chem.\nEng."},{"issue":"7","key":"2026092210580951900_cit2","doi-asserted-by":"publisher","first-page":"1694","DOI":"10.3390\/polym15071694","article-title":"The Biomodified\nLignin Platform: A Review","volume":"15","author":"Fabbri","year":"2023","journal-title":"Polymers"},{"issue":"22","key":"2026092210580951900_cit3","doi-asserted-by":"publisher","first-page":"8086","DOI":"10.1021\/ACSSUSCHEMENG.0C01348","article-title":"Perspective\non Technical Lignin Fractionation","volume":"8","author":"Sadeghifar","year":"2020","journal-title":"ACS Sustainable\nChem. Eng."},{"key":"2026092210580951900_cit4","doi-asserted-by":"publisher","first-page":"979","DOI":"10.1016\/j.ijbiomac.2017.08.102","article-title":"Aqueous Acetone Fractionation of\nKraft, Organosolv and Soda Lignins","volume":"106","author":"Domi\u0301nguez-Robles","year":"2018","journal-title":"Int. J.\nBiol. Macromol."},{"issue":"11","key":"2026092210580951900_cit5","doi-asserted-by":"publisher","first-page":"10112","DOI":"10.1021\/acssuschemeng.9b01641","article-title":"Using Green \u03b3-Valerolactone\/Water\nSolvent To Decrease Lignin\nHeterogeneity by Gradient Precipitation","volume":"7","author":"Wang","year":"2019","journal-title":"ACS\nSustainable Chem. Eng."},{"issue":"12","key":"2026092210580951900_cit6","doi-asserted-by":"publisher","first-page":"2893","DOI":"10.3390\/molecules25122893","article-title":"Tuning Lignin\nCharacteristics by Fractionation: A Versatile Approach Based on Solvent\nExtraction and Membrane-Assisted Ultrafiltration","volume":"25","author":"Allegretti","year":"2020","journal-title":"Molecules"},{"issue":"3","key":"2026092210580951900_cit7","doi-asserted-by":"publisher","first-page":"4615","DOI":"10.1021\/acsomega.8b02851","article-title":"Two-Step Fractionation\nof a Model Technical Lignin by Combined Organic Solvent Extraction\nand Membrane Ultrafiltration","volume":"4","author":"Allegretti","year":"2019","journal-title":"ACS Omega"},{"key":"2026092210580951900_cit8","doi-asserted-by":"publisher","first-page":"480","DOI":"10.1016\/j.ijbiomac.2020.07.153","article-title":"Efficient\nDissolution of Lignin in Novel Ternary Deep Eutectic Solvents\nand Its Application in Polyurethane","volume":"164","author":"Xue","year":"2020","journal-title":"Int. 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Macromol."},{"issue":"12","key":"2026092210580951900_cit14","doi-asserted-by":"publisher","first-page":"2334","DOI":"10.3390\/MOLECULES24122334","article-title":"Modeling of Solid\u2013Liquid Equilibria\nin Deep Eutectic Solvents: A Parameter Study","volume":"24","author":"Alhadid","year":"2019","journal-title":"Molecules"},{"issue":"21","key":"2026092210580951900_cit15","doi-asserted-by":"publisher","first-page":"11060","DOI":"10.1021\/cr300162p","article-title":"Deep Eutectic\nSolvents (DESs) and\nTheir Applications","volume":"114","author":"Smith","year":"2014","journal-title":"Chem. 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Eng."},{"key":"2026092210580951900_cit26","doi-asserted-by":"publisher","first-page":"102190","DOI":"10.1016\/j.biteb.2025.102190","article-title":"Deep Eutectic Solvents (DESs) in\nLignocellulosic Biomass\nPretreatment: Mechanisms and Process Optimization","volume":"31","author":"Arshad","year":"2025","journal-title":"Bioresour. Technol. Rep."},{"key":"2026092210580951900_cit27","doi-asserted-by":"publisher","first-page":"120853","DOI":"10.1016\/j.seppur.2022.120853","article-title":"Systematic Method of Screening Deep Eutectic Solvents\nas Extractive\nSolvents for M-Cresol\/Cumene Separation","volume":"291","author":"Liu","year":"2022","journal-title":"Sep.\nPurif. Technol."},{"key":"2026092210580951900_cit28","doi-asserted-by":"publisher","first-page":"113361","DOI":"10.1016\/j.molliq.2020.113361","article-title":"ATR-IR Spectroscopy for Rapid Quantification of Water\nContent in Deep Eutectic Solvents","volume":"311","author":"Elderderi","year":"2020","journal-title":"J. Mol. Liq."},{"key":"2026092210580951900_cit29","doi-asserted-by":"publisher","first-page":"108805","DOI":"10.1016\/j.jmgm.2024.108805","article-title":"Combined Experimental\nand Computational\nInvestigation of Tetrabutylammonium Bromide-Carboxylic Acid-Based\nDeep Eutectic Solvents","volume":"131","author":"Shokri","year":"2024","journal-title":"J. Mol. Graphics Modell."},{"issue":"69","key":"2026092210580951900_cit30","doi-asserted-by":"publisher","first-page":"10253","DOI":"10.1039\/C9CC04846D","article-title":"Phenolic Hydrogen\nBond Donors in\nthe Formation of Non-Ionic Deep Eutectic Solvents: The Quest for Type\nv Des","volume":"55","author":"Abranches","year":"2019","journal-title":"Chem. Commun."},{"issue":"3","key":"2026092210580951900_cit31","doi-asserted-by":"publisher","first-page":"551","DOI":"10.1134\/S0036024420020028","article-title":"Calculation and Experimental Studies\nof Systems of Dibasic Carboxylic Acids and Properties of Eutectics","volume":"94","author":"Alenova","year":"2020","journal-title":"Russ. J. Phys. Chem. A"},{"issue":"28","key":"2026092210580951900_cit32","doi-asserted-by":"publisher","first-page":"8360","DOI":"10.1039\/D4GC06386D","article-title":"Natural Deep Eutectic\nSolvents (NaDES)","volume":"27","author":"Cheve\u0301-Kools","year":"2025","journal-title":"Green Chem."},{"issue":"2","key":"2026092210580951900_cit33","doi-asserted-by":"publisher","first-page":"275","DOI":"10.1039\/C8GC03064B","article-title":"Facile\nFractionation of Lignocelluloses\nby Biomass-Derived Deep Eutectic Solvent (DES) Pretreatment for Cellulose\nEnzymatic Hydrolysis and Lignin Valorization","volume":"21","author":"Shen","year":"2019","journal-title":"Green Chem."},{"issue":"8","key":"2026092210580951900_cit34","doi-asserted-by":"publisher","first-page":"2474","DOI":"10.1039\/C9GC02569C","article-title":"Novel\nInsights into Biomass Delignification with Acidic Deep Eutectic Solvents:\nA Mechanistic Study of \u03b2-O-4 Ether Bond Cleavage and the Role\nof the Halide Counterion in the Catalytic Performance","volume":"22","author":"Da Costa Lopes","year":"2020","journal-title":"Green Chem."},{"key":"2026092210580951900_cit35","doi-asserted-by":"publisher","first-page":"112241","DOI":"10.1016\/j.indcrop.2020.112241","article-title":"Lignin Extraction and Upgrading Using\nDeep Eutectic Solvents","volume":"147","author":"Chen","year":"2020","journal-title":"Ind. 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Technol."},{"key":"2026092210580951900_cit38","doi-asserted-by":"publisher","first-page":"126","DOI":"10.1016\/j.carbon.2015.12.078","article-title":"Processing and Characterization\nof Low-Cost Electrospun Carbon Fibers from Organosolv Lignin\/Polyacrylonitrile\nBlends","volume":"100","author":"Ding","year":"2016","journal-title":"Carbon"},{"issue":"1","key":"2026092210580951900_cit39","doi-asserted-by":"publisher","first-page":"10","DOI":"10.12691\/jpbpc-10-1-2","article-title":"An Experimental Review:\nEvaluation of the Flory-Fox\nEquation for the Relationship of Glass Transition Temperature (Tg) vs Molar Mass of Polystyrene Using Differential Scanning\nCalorimetry (DSC)","volume":"10","author":"D\u2019amelia","year":"2022","journal-title":"J. Polym. Biopolym. Phys.\nChem."},{"key":"2026092210580951900_cit40","doi-asserted-by":"publisher","first-page":"793","DOI":"10.1016\/j.ijbiomac.2017.08.069","article-title":"Fractionation of\nLignin Macromolecules by Sequential Organic Solvents Systems and Their\nCharacterization for Further Valuable Applications","volume":"106","author":"Park","year":"2018","journal-title":"Int. J. Biol. Macromol."},{"issue":"10","key":"2026092210580951900_cit41","doi-asserted-by":"publisher","first-page":"20682","DOI":"10.3390\/IJMS141020682","article-title":"Thermal Properties\nand Crystallite\nMorphology of Nylon 66 Modified with a Novel Biphenyl Aromatic Liquid\nCrystalline Epoxy Resin","volume":"14","author":"Cai","year":"2013","journal-title":"Int. J. Mol. Sci."},{"key":"2026092210580951900_cit42","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1051\/mfreview\/2016020","article-title":"Production and 3D Printing Processing\nof Bio-Based Thermoplastic Filament","volume":"4","author":"Gkartzou","year":"2017","journal-title":"Manuf.\nRev."},{"key":"2026092210580951900_cit43","doi-asserted-by":"publisher","first-page":"100106","DOI":"10.1016\/j.crgsc.2021.100106","article-title":"Thermal\nand Structural Characterization of Two Commercially\nAvailable Technical Lignins for Potential Depolymerization via Hydrothermal\nLiquefaction","volume":"4","author":"Amit","year":"2021","journal-title":"Curr. Res. Green Sustainable Chem."},{"issue":"3","key":"2026092210580951900_cit44","doi-asserted-by":"publisher","first-page":"4239","DOI":"10.15376\/biores.10.3.4239-4251","article-title":"TGA-FTIR Analysis\nof Torrefaction\nof Lignocellulosic Components (Cellulose, Xylan, Lignin) in Isothermal\nConditions over a Wide Range of Time Durations","volume":"10","author":"Lv","year":"2015","journal-title":"BioResources"},{"issue":"4","key":"2026092210580951900_cit45","doi-asserted-by":"publisher","first-page":"1627","DOI":"10.1021\/acs.biomac.2c01356","article-title":"The Glass Transition\nTemperature of Heterogeneous Biopolymer Systems","volume":"24","author":"Espi\u0301ndola","year":"2023","journal-title":"Biomacromolecules"},{"key":"2026092210580951900_cit46","doi-asserted-by":"publisher","first-page":"126528","DOI":"10.1016\/j.biortech.2021.126528","article-title":"Microwave-Assisted\nExtraction of\nLignin from Coconut Coir Using Deep Eutectic Solvents and Its Valorization\nto Aromatics","volume":"345","author":"Mankar","year":"2022","journal-title":"Bioresour. Technol."},{"key":"2026092210580951900_cit47","doi-asserted-by":"publisher","first-page":"120476","DOI":"10.1016\/j.indcrop.2025.120476","article-title":"Depolymerization and\nProduct Evolution of Kraft Lignin in a Novel\nAcid Deep Eutectic Solvents (DESs)","volume":"225","author":"Li","year":"2025","journal-title":"Ind. Crops\nProd."},{"issue":"8","key":"2026092210580951900_cit48","doi-asserted-by":"publisher","first-page":"1942","DOI":"10.1039\/D3SE00045A","article-title":"Structure Elucidation\nof Prot, Alkali and Dealkaline\nLignin(s) by NMR, FT-IR and Py-GC\/MS: Effect of Solid Acid and Base\nCatalysts","volume":"7","author":"Kumar","year":"2023","journal-title":"Sustainable Energy Fuels"},{"issue":"16","key":"2026092210580951900_cit49","doi-asserted-by":"publisher","DOI":"10.1002\/CSSC.202500607","article-title":"Nitrogen-Functionalized Lignin: Current\nStatus, Applications, and Challenges","volume":"18","author":"Chen","year":"2025","journal-title":"ChemSusChem"},{"issue":"4","key":"2026092210580951900_cit50","doi-asserted-by":"publisher","first-page":"5401","DOI":"10.1007\/S13399-024-05622-1","article-title":"Bio-Oil as a Source\nof Renewable Chemicals: The Chemistry of Pyrolytic Lignin","volume":"15","author":"Silva","year":"2024","journal-title":"Biomass Convers. 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