{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T15:55:22Z","timestamp":1791474922195,"version":"4.3.4"},"reference-count":40,"publisher":"MDPI AG","issue":"19","license":[{"start":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T00:00:00Z","timestamp":1791417600000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"},{"start":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T00:00:00Z","timestamp":1791417600000},"content-version":"tdm","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Polymers"],"abstract":"<jats:p>To address the poor adhesion of waterborne inks to polyethylene terephthalate (PET) films, a low-temperature ketone\u2013hydrazide self-crosslinking system based on 2-(acetoacetoxy)ethyl methacrylate (AAEM) and adipic acid dihydrazide (ADH) was incorporated into a waterborne polyurethane\u2013acrylate emulsion. Self-crosslinking waterborne polyurethane\u2013acrylate emulsions (AWPUAs) with different AAEM contents were prepared and subsequently used as binders in waterborne inks for PET films. The results showed that increasing the AAEM content reduced the water absorption of the latex films while increasing their water contact angle and tensile strength. Meanwhile, the adhesion of the resulting waterborne inks to corona-treated PET films increased with increasing AAEM content, together with a substantial enhancement in re-solubility. At an AAEM content of 7 wt%, the AWPUA emulsion exhibited good colloidal stability, and the corresponding waterborne ink achieved nearly 100% adhesion while maintaining good re-solubility. These findings demonstrate that AAEM\/ADH ketone\u2013hydrazide self-crosslinking modification provides an effective approach for improving the film properties of waterborne polyurethane\u2013acrylate emulsions and the application performance of waterborne inks on PET films.<\/jats:p>","DOI":"10.3390\/polym18192453","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T15:16:52Z","timestamp":1791472612000},"page":"2453","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["AAEM\/ADH Self-Crosslinking Waterborne Polyurethane\u2013Acrylate Binder for High-Adhesion Waterborne Inks on PET Films"],"prefix":"10.3390","volume":"18","author":[{"given":"Junqing","family":"Xi","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering, North University of China, Taiyuan 030051, China"},{"name":"Dezhou Industrial Technology Research Institute of North University of China, Dezhou 253034, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"methodology","vocabulary":"credit"},{"role":"formal-analysis","vocabulary":"credit"},{"role":"writing-original-draft","vocabulary":"credit"}]},{"given":"Chenglong","family":"Jiao","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering, North University of China, Taiyuan 030051, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"visualization","vocabulary":"credit"},{"role":"data-curation","vocabulary":"credit"}]},{"given":"Chao","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering, North University of China, Taiyuan 030051, China"},{"name":"Dezhou Industrial Technology Research Institute of North University of China, Dezhou 253034, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"investigation","vocabulary":"credit"}]},{"given":"Shixiong","family":"Sun","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering, North University of China, Taiyuan 030051, China"},{"name":"Dezhou Industrial Technology Research Institute of North University of China, Dezhou 253034, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"investigation","vocabulary":"credit"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-0848-9874","authenticated-orcid":false,"given":"Benbo","family":"Zhao","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering, North University of China, Taiyuan 030051, China"},{"name":"Dezhou Industrial Technology Research Institute of North University of China, Dezhou 253034, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"conceptualization","vocabulary":"credit"},{"role":"writing-review-editing","vocabulary":"credit"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6927-2635","authenticated-orcid":false,"given":"Yunjun","family":"Luo","sequence":"additional","affiliation":[{"name":"School of Materials Science and Technology, Beijing Institute of Technology, Beijing 100081, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"conceptualization","vocabulary":"credit"},{"role":"writing-review-editing","vocabulary":"credit"}]}],"member":"1968","published-online":{"date-parts":[[2026,10,8]]},"reference":[{"key":"ref_1","first-page":"108320","article-title":"Recent advancement in synthesis and modification of water-based acrylic emulsion and their application in water-based ink: A comprehensive review","volume":"189","author":"Tian","year":"2024","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_2","doi-asserted-by":"crossref","first-page":"1569","DOI":"10.1002\/pen.25681","article-title":"Synthesis of waterborne acrylic copolymer resin as a binding agent for the development of water-based inks in the printing application","volume":"61","author":"Sharma","year":"2021","journal-title":"Polym. Eng. Sci."},{"key":"ref_3","first-page":"105190","article-title":"Synthesis and characterization of multiple-crosslinkable polyacrylate emulsion for PVC film ink","volume":"138","author":"Gao","year":"2020","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_4","doi-asserted-by":"crossref","unstructured":"Li, M., Wang, Y., Ye, J., Guo, L., and Wang, H. (2025). Synthesis of Crosslinkable Alkali-Soluble Resins and Self-Crosslinking Polyacrylic Latexes. Molecules, 30.","DOI":"10.3390\/molecules30122551"},{"key":"ref_5","first-page":"66","article-title":"Synthesis and characterization of low-temperature self-crosslinkable acrylic emulsion for PE film ink","volume":"81","author":"Pi","year":"2015","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_6","first-page":"107765","article-title":"Enhancement of the adhesion strength of water-based ink binder based on waterborne polyurethane","volume":"183","author":"Zhao","year":"2023","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_7","first-page":"105298","article-title":"Synthesis and application of acrylate copolymer as high ink-absorption and fast drying coating agent for polyester fabric","volume":"136","author":"Liu","year":"2019","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_8","doi-asserted-by":"crossref","unstructured":"Izdebska-Podsiad\u0142y, J., and Napi\u00f3rkowska, J. (2023). Effect of Aminopropyltriethoxysilane on the Adhesion of Flexographic Water-Based Ink to Packaging Films. Coatings, 13.","DOI":"10.3390\/coatings13111833"},{"key":"ref_9","doi-asserted-by":"crossref","first-page":"489","DOI":"10.1002\/col.22579","article-title":"Surface analysis of polymer films for wettability and ink adhesion","volume":"46","author":"Aydemir","year":"2020","journal-title":"Color. Res. Appl."},{"key":"ref_10","first-page":"161","article-title":"Preparation and properties of a novel low crystallinity cross-linked network waterborne polyurethane for water-based ink","volume":"133","author":"Zhu","year":"2019","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_11","first-page":"61","article-title":"Synthesis and characterization of low crystalline waterborne polyurethane for potential application in water-based ink binder","volume":"77","author":"Fang","year":"2014","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_12","doi-asserted-by":"crossref","first-page":"708","DOI":"10.1016\/j.jmst.2015.03.002","article-title":"Recent Advances in Synthesis of Waterborne Polyurethane and Their Application in Water-based Ink: A Review","volume":"31","author":"Zhou","year":"2015","journal-title":"J. Mater. Sci. Technol."},{"key":"ref_13","doi-asserted-by":"crossref","unstructured":"Liu, X., Hong, W., and Chen, X. (2020). Continuous Production of Water-Borne Polyurethanes: A Review. Polymers, 12.","DOI":"10.3390\/polym12122875"},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"2443","DOI":"10.1021\/acsomega.0c05593","article-title":"Advances in Waterborne Acrylic Resins: Synthesis Principle, Modification Strategies, and Their Applications","volume":"6","author":"Jiao","year":"2021","journal-title":"ACS Omega"},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"427","DOI":"10.1515\/epoly-2014-0163","article-title":"UV-curable electromagnetic shielding composite films produced through waterborne polyurethane-acrylate bonded graphene oxide: Preparation and effect of different diluents on the properties","volume":"14","author":"Dai","year":"2014","journal-title":"e-Polymers"},{"key":"ref_16","doi-asserted-by":"crossref","unstructured":"Luo, Q., Wen, X., Xu, R., Liu, Z., Xiang, H., Li, Z., and Liu, X. (2022). Preparation and Properties of Novel Modified Waterborne Polyurethane Acrylate. Coatings, 12.","DOI":"10.3390\/coatings12081135"},{"key":"ref_17","doi-asserted-by":"crossref","first-page":"855","DOI":"10.1007\/s11998-025-01173-w","article-title":"Eco-friendly waterborne polyurethane acrylates: Incorporating itaconic acid-derived epoxy acrylates for advanced coatings","volume":"23","author":"Kim","year":"2025","journal-title":"J. Coat. Technol. Res."},{"key":"ref_18","doi-asserted-by":"crossref","unstructured":"Chen, X., Ye, X., Lu, L., Qian, Y., Wang, L., Bi, Y., Wang, Z., and Cai, Z. (2020). Preparation of Cross-Linkable Waterborne Polyurethane-Acrylate Coating Films with Multifunctional Properties. Coatings, 10.","DOI":"10.3390\/coatings10010065"},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"887","DOI":"10.1016\/j.dental.2026.01.011","article-title":"Development of a new dental resin matrix using a fluorinated urethane acrylate monomer","volume":"42","author":"Yang","year":"2026","journal-title":"Dent. Mater."},{"key":"ref_20","first-page":"109376","article-title":"Enhanced adhesion to low-surface-energy substrates using polyurethane acrylate\/polyacrylate interpenetrating network pressure-sensitive adhesives","volume":"206","author":"Han","year":"2025","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_21","first-page":"110188","article-title":"Low-viscosity polyurethane acrylate based on hydrogen bond dissociation and its effect on the mechanical properties of materials","volume":"216","author":"Chen","year":"2026","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_22","first-page":"109081","article-title":"Preparation and properties of core-shell self-matting waterborne polyurethane acrylate","volume":"200","author":"Yang","year":"2025","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_23","first-page":"107767","article-title":"High solid and low viscosity waterborne polyurethane acrylate with excellent anti-corrosion and anti-bacterial performances","volume":"183","author":"Chen","year":"2023","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_24","doi-asserted-by":"crossref","unstructured":"Wang, X., Wu, J., Chu, F., and Feng, Y. (2022). Preparation of Polyurethane\/Acrylate Composite Emulsion for Inkjet Printing. Coatings, 12.","DOI":"10.3390\/coatings12081081"},{"key":"ref_25","first-page":"108372","article-title":"Organosilicon-modified double crosslinked waterborne polyurethane coatings","volume":"190","author":"Xing","year":"2024","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_26","first-page":"105543","article-title":"Polyurethane modified epoxy acrylate resins containing \u03b5-caprolactone unit","volume":"141","author":"Xu","year":"2020","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_27","doi-asserted-by":"crossref","first-page":"5517","DOI":"10.1007\/s00289-018-2666-6","article-title":"Synthesis and surface migration of polydimethylsiloxane and perfluorinated polyether in modified waterborne polyurethane","volume":"76","author":"Zhang","year":"2019","journal-title":"Polym. Bull."},{"key":"ref_28","doi-asserted-by":"crossref","first-page":"6791","DOI":"10.2147\/IJN.S393207","article-title":"Biological Effects, Applications and Design Strategies of Medical Polyurethanes Modified by Nanomaterials","volume":"17","author":"Wang","year":"2022","journal-title":"Int. J. Nanomed."},{"key":"ref_29","doi-asserted-by":"crossref","first-page":"112062","DOI":"10.1016\/j.mtcomm.2025.112062","article-title":"Construction of waterborne polyurethane crosslinking network with excellent adhesion strength, mechanical properties, and wear resistance","volume":"44","author":"Zhang","year":"2025","journal-title":"Mater. Today Commun."},{"key":"ref_30","first-page":"108386","article-title":"A rapid room-temperature self-healing, antibacterial, photoluminescent waterborne polyurethane coating with excellent mechanical properties based on double dynamic cross-linked network used for leather finishing","volume":"190","author":"Li","year":"2024","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_31","doi-asserted-by":"crossref","first-page":"2742","DOI":"10.1039\/D1MH01217G","article-title":"An unparalleled H-bonding and ion-bonding crosslinked waterborne polyurethane with super toughness and unprecedented fracture energy","volume":"8","author":"Yao","year":"2021","journal-title":"Mater. Horiz."},{"key":"ref_32","first-page":"107578","article-title":"Crosslinking of waterborne polyurethane using dibromide as a crosslinker and 1,1,3,3-tetramethylguanidine (TMG) as an esterification promotor","volume":"181","author":"Kai","year":"2023","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_33","first-page":"108174","article-title":"Pickering emulsion approach: A novel strategy to fabricate waterborne polyurethane with enhanced abradability and water-resistance comparable to that of solvent-based coating","volume":"188","author":"Wu","year":"2024","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_34","doi-asserted-by":"crossref","first-page":"130897","DOI":"10.1016\/j.conbuildmat.2023.130897","article-title":"Study of keto-hydrazide crosslinking effect in acrylic latex applied to Portland cements with respect to physical properties","volume":"375","author":"Viani","year":"2023","journal-title":"Constr. Build. Mater."},{"key":"ref_35","first-page":"108776","article-title":"Synthesis of acrylic water-based inks for plastic films: Tuning binder\u2019s properties by low temperature self-crosslinking of allyl acetoacetate-hexamethylenediamine","volume":"197","author":"Tian","year":"2024","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_36","doi-asserted-by":"crossref","first-page":"113693","DOI":"10.1016\/j.dyepig.2026.113693","article-title":"Enhanced adhesion and drying performance: DAAM\/ADH crosslinked acrylate emulsion modified by low acid value alkali-soluble resin and its influence on water-based ink properties","volume":"251","author":"Ma","year":"2026","journal-title":"Dye. Pigment."},{"key":"ref_37","first-page":"108851","article-title":"Effects of ASRs, alkali neutralizers and crosslinking reaction on the application properties of self-crosslinking polyacrylate latex binders","volume":"197","author":"Li","year":"2024","journal-title":"Prog. Progress. Org. Coat."},{"key":"ref_38","doi-asserted-by":"crossref","first-page":"1644","DOI":"10.1021\/acs.iecr.5c04490","article-title":"Self-Cross-Linking Hybrid Protein-Acrylic Latexes through the Keto-Hydrazide Reaction","volume":"65","author":"Parra","year":"2026","journal-title":"Ind. Eng. Chem. Res."},{"key":"ref_39","doi-asserted-by":"crossref","first-page":"14820","DOI":"10.1021\/acssuschemeng.8b03349","article-title":"Reduced Graphene Oxide Reinforced Waterborne Soy Alkyd Nanocomposites: Formulation, Characterization, and Corrosion Inhibition Analysis","volume":"6","author":"Irfan","year":"2018","journal-title":"ACS Sustain. Chem. Eng."},{"key":"ref_40","doi-asserted-by":"crossref","first-page":"170","DOI":"10.1016\/j.indcrop.2019.04.039","article-title":"Synthesis and characterization of a novel tri-functional bio-based methacrylate prepolymer from castor oil and its application in UV-curable coatings","volume":"135","author":"Liang","year":"2019","journal-title":"Ind. Crops Prod."}],"container-title":["Polymers"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/2073-4360\/18\/19\/2453\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T15:22:08Z","timestamp":1791472928000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/2073-4360\/18\/19\/2453"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,10,8]]},"references-count":40,"journal-issue":{"issue":"19","published-online":{"date-parts":[[2026,10]]}},"alternative-id":["polym18192453"],"URL":"https:\/\/doi.org\/10.3390\/polym18192453","relation":{},"ISSN":["2073-4360"],"issn-type":[{"value":"2073-4360","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,10,8]]}}}