{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T12:06:44Z","timestamp":1789992404912,"version":"4.0.1"},"reference-count":40,"publisher":"MDPI AG","issue":"18","license":[{"start":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T00:00:00Z","timestamp":1789948800000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["22075288"],"award-info":[{"award-number":["22075288"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]},{"award":["22075288"],"award-info":[{"award-number":["22075288"]}],"id":[{"id":"https:\/\/ror.org\/01h0zpd94","id-type":"ROR","asserted-by":"publisher"}]},{"name":"Key\u2013Area Research Program for General Higher Education Institutions of Guangdong Province","award":["2024ZDZX3036"],"award-info":[{"award-number":["2024ZDZX3036"]}]},{"name":"Guangzhou Municipal Bureau of Education University Scientific Research Project","award":["2024312482"],"award-info":[{"award-number":["2024312482"]}]},{"name":"The Science and Technology Program of Hunan Province","award":["2024AQ2013"],"award-info":[{"award-number":["2024AQ2013"]}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Polymers"],"abstract":"<jats:p>A poly (acrylic acid\u2013tannic acid) (PAA\u2013TA) crosslinked composite is reported on for the first time as an aqueous binder for LiMn0.6Fe0.4PO4 (LMFP) cathodes to suppress manganese dissolution. Benefiting from hydrogen bonding and chemical crosslinking, the PAA-TA binder constructs a robust three-dimensional network that strengthens the interfacial adhesion among active particles, conductive additives, and the current collector, stabilizing the LMFP crystal structure upon cycling. More importantly, this polymeric network effectively restrains manganese leaching, which is the major origin of the capacity fading of LMFP cathodes. Meanwhile, continuous electron and ion transport pathways are well established. The LMFP electrode with an optimized PA5TA1 binder delivers a reversible capacity of 112 mAh g\u22121 at 5 C and retains 81.3% of its capacity after 300 cycles, outperforming the PVDF\/LMFP electrode. Post\u2013mortem analyses of cycled LMFP cathodes further confirm that there was substantially suppressed Mn2+ dissolution in the PAA\u2013TA electrode, corroborating the structural integrity of the cathode\u2013electrolyte interface. This crosslinked aqueous polymer provides a sustainable alternative to the PVDF binder for long\u2013life LMFP cathodes.<\/jats:p>","DOI":"10.3390\/polym18182308","type":"journal-article","created":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T11:05:53Z","timestamp":1789988753000},"page":"2308","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Multifunctional Crosslinked PAA\u2013TA Binder: Robust Structural Integrity and Suppressed Manganese Dissolution for High\u2013Performance LiMn0.6Fe0.4PO4 Cathodes"],"prefix":"10.3390","volume":"18","author":[{"given":"Jiajun","family":"Zhou","sequence":"first","affiliation":[{"name":"School of Marine Equipment Engineering, Guangzhou Maritime University, Guangzhou 510725, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"writing-original-draft","vocabulary":"credit"},{"role":"methodology","vocabulary":"credit"},{"role":"visualization","vocabulary":"credit"},{"role":"investigation","vocabulary":"credit"},{"role":"data-curation","vocabulary":"credit"}]},{"given":"Weibin","family":"Zhao","sequence":"additional","affiliation":[{"name":"School of Marine Equipment Engineering, Guangzhou Maritime University, Guangzhou 510725, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"software","vocabulary":"credit"},{"role":"methodology","vocabulary":"credit"},{"role":"data-curation","vocabulary":"credit"},{"role":"visualization","vocabulary":"credit"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3106-9348","authenticated-orcid":false,"given":"Jinchang","family":"Xu","sequence":"additional","affiliation":[{"name":"Guangdong Provincial Key Laboratory of Terahertz Quantum Electromagnetics, GBA Branch of Aerospace Information Research Institute, Chinese Academy of Sciences, Guangzhou 510700, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"data-curation","vocabulary":"credit"},{"role":"validation","vocabulary":"credit"}]},{"given":"Yue","family":"Li","sequence":"additional","affiliation":[{"name":"School of Marine Equipment Engineering, Guangzhou Maritime University, Guangzhou 510725, China"},{"name":"School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"validation","vocabulary":"credit"},{"role":"methodology","vocabulary":"credit"}]},{"given":"Fenghao","family":"Zheng","sequence":"additional","affiliation":[{"name":"School of Marine Equipment Engineering, Guangzhou Maritime University, Guangzhou 510725, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"methodology","vocabulary":"credit"},{"role":"validation","vocabulary":"credit"}]},{"given":"Aiguo","family":"Chen","sequence":"additional","affiliation":[{"name":"School of Marine Equipment Engineering, Guangzhou Maritime University, Guangzhou 510725, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"funding-acquisition","vocabulary":"credit"},{"role":"writing-review-editing","vocabulary":"credit"},{"role":"project-administration","vocabulary":"credit"}]},{"given":"Junjie","family":"Tong","sequence":"additional","affiliation":[{"name":"School of Marine Equipment Engineering, Guangzhou Maritime University, Guangzhou 510725, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"writing-review-editing","vocabulary":"credit"},{"role":"software","vocabulary":"credit"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2443-6023","authenticated-orcid":false,"given":"Yangxi","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Marine Equipment Engineering, Guangzhou Maritime University, Guangzhou 510725, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"writing-review-editing","vocabulary":"credit"},{"role":"project-administration","vocabulary":"credit"},{"role":"formal-analysis","vocabulary":"credit"}]},{"given":"Haoxiang","family":"Zhong","sequence":"additional","affiliation":[{"name":"School of Marine Equipment Engineering, Guangzhou Maritime University, Guangzhou 510725, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"conceptualization","vocabulary":"credit"},{"role":"formal-analysis","vocabulary":"credit"},{"role":"investigation","vocabulary":"credit"},{"role":"resources","vocabulary":"credit"},{"role":"supervision","vocabulary":"credit"},{"role":"project-administration","vocabulary":"credit"},{"role":"funding-acquisition","vocabulary":"credit"},{"role":"writing-review-editing","vocabulary":"credit"}]}],"member":"1968","published-online":{"date-parts":[[2026,9,21]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"115971","DOI":"10.1016\/j.rser.2025.115971","article-title":"Lithium-Ion Batteries and the Future of Sustainable Energy: A Comprehensive Review","volume":"223","author":"Ngoy","year":"2025","journal-title":"Renew. Sustain. Energy Rev."},{"key":"ref_2","doi-asserted-by":"crossref","first-page":"40399","DOI":"10.1039\/D5TA03194J","article-title":"Emerging Multimetal LMFP-based Cathodes for Lithium-Ion Batteries: A Review","volume":"13","author":"Mubarac","year":"2025","journal-title":"J. Mater. Chem. A"},{"key":"ref_3","doi-asserted-by":"crossref","first-page":"112552","DOI":"10.1016\/j.est.2024.112552","article-title":"Providing High Stability to Suppress Metal Dissolution in LiMn0.5Fe0.5PO4 Cathode Materials by Zn Doping","volume":"96","author":"Jeong","year":"2024","journal-title":"J. Energy Stor."},{"key":"ref_4","doi-asserted-by":"crossref","first-page":"7072","DOI":"10.1021\/acsaem.5c00437","article-title":"Revealing the Role of Carbon Layers in Lithium Manganese Iron Phosphate Cathodes: Synergistic Enhancement of Interfacial Charge Transport and Structural Stability","volume":"8","author":"Bing","year":"2025","journal-title":"ACS Appl. Energy Mater."},{"key":"ref_5","doi-asserted-by":"crossref","first-page":"500118","DOI":"10.20517\/energymater.2025.29","article-title":"Lithium Manganese Iron Phosphate (LiMn1-y Fey PO4) Rechargeable Batteries: Bridging Material Innovation with Practical Cell Design","volume":"5","author":"Jung","year":"2025","journal-title":"Energy Mater."},{"key":"ref_6","doi-asserted-by":"crossref","first-page":"2400814","DOI":"10.1002\/adsu.202400814","article-title":"Achieving Fast Mn Redox Kinetics with Solvothermal Synthesized (010) Facet Preferential LiMn0.5 Fe0.5 PO4 Nanoplates for Li-Ion Batteries","volume":"9","author":"Lin","year":"2025","journal-title":"Adv. Sustain. Syst."},{"key":"ref_7","doi-asserted-by":"crossref","first-page":"9","DOI":"10.1007\/s40820-025-01848-4","article-title":"Tackling Challenges and Exploring Opportunities in Cathode Binder Innovation","volume":"18","author":"Lai","year":"2026","journal-title":"Nano-Micro Lett."},{"key":"ref_8","doi-asserted-by":"crossref","first-page":"194","DOI":"10.1016\/j.pnsc.2024.02.013","article-title":"Progress and Challenges for Replacing N-Methyl-2-Pyrrolidone\/Polyvinylidene Fluoride Slurry Formulations in Lithium-Ion Battery Cathodes","volume":"34","author":"Mun","year":"2024","journal-title":"Prog. Nat. Sci. Mater. Int."},{"key":"ref_9","doi-asserted-by":"crossref","first-page":"e202501943","DOI":"10.1002\/cssc.202501943","article-title":"Fluorine-Free Binder Strategies for High-Nickel Cathodes: Toward PFAS-Free Lithium-Ion Batteries","volume":"19","author":"Shin","year":"2026","journal-title":"ChemSusChem"},{"key":"ref_10","doi-asserted-by":"crossref","first-page":"100838","DOI":"10.1016\/j.ceja.2025.100838","article-title":"Advanced Cathode Binders for Lithium-Ion Batteries: Molecular Design and Performance Enhancement","volume":"24","author":"Tian","year":"2025","journal-title":"Chem. Eng. J. Adv."},{"key":"ref_11","doi-asserted-by":"crossref","first-page":"4047","DOI":"10.1021\/acsaem.1c02923","article-title":"Suitable Cathode NMP Replacement for Efficient Sustainable Printed Li-Ion Batteries","volume":"5","author":"Sliz","year":"2022","journal-title":"ACS Appl. Energy Mater."},{"key":"ref_12","doi-asserted-by":"crossref","first-page":"154933","DOI":"10.1016\/j.apsusc.2022.154933","article-title":"Poly (hydroxybutyrate-co-hydroxyvalerate) as a Biodegradable Binder in a Negative Electrode Material for Lithium-Ion Batteries","volume":"606","author":"Nowak","year":"2022","journal-title":"Appl. Surf. Sci."},{"key":"ref_13","doi-asserted-by":"crossref","unstructured":"Dobryden, I., Montanari, C., Bhattacharjya, D., Aydin, J., and Ahniyaz, A. (2023). Bio-Based Binder Development for Lithium-Ion Batteries. Materials, 16.","DOI":"10.3390\/ma16165553"},{"key":"ref_14","doi-asserted-by":"crossref","first-page":"9430","DOI":"10.1021\/acsaem.5c01008","article-title":"Novel Copolymer Dispersant with Promoted Dispersibility of the LMFP Cathode Slurry for Boosting the Li-Ion Battery Performance","volume":"8","author":"Pan","year":"2025","journal-title":"ACS Appl. Energy Mater."},{"key":"ref_15","doi-asserted-by":"crossref","first-page":"7952","DOI":"10.1039\/C7TA00104E","article-title":"Effects of Adhesives on the Electrochemical Performance of Monodisperse LiMn0.8 Fe0.2 PO4\/C Microspheres as Cathode Materials for High Power Lithium-Ion Batteries","volume":"5","author":"Li","year":"2017","journal-title":"J. Mater. Chem. A"},{"key":"ref_16","doi-asserted-by":"crossref","first-page":"36697","DOI":"10.1021\/acsami.9b12113","article-title":"High-Rate Structure-Gradient Ni-Rich Cathode Material for Lithium-Ion Batteries","volume":"11","author":"Su","year":"2019","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_17","doi-asserted-by":"crossref","first-page":"51808","DOI":"10.1021\/acsami.2c11695","article-title":"Sulfated Alginate as an Effective Polymer Binder for High-Voltage LiNi0.5 Mn1.5 O4 Electrodes in Lithium-Ion Batteries","volume":"14","author":"Oishi","year":"2022","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_18","doi-asserted-by":"crossref","first-page":"861","DOI":"10.1021\/acsami.1c19554","article-title":"Multifunctional Composite Binder for Thick High-Voltage Cathodes in Lithium-Ion Batteries","volume":"14","author":"Rao","year":"2022","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_19","doi-asserted-by":"crossref","first-page":"239006","DOI":"10.1016\/j.jpowsour.2025.239006","article-title":"PAA\/HNBR Composite Binder: A Sustainable Fluorine-Free Binder Strategy for High-Rate and Durable LiFePO4 Cathodes","volume":"665","author":"Duan","year":"2026","journal-title":"J. Power Sources"},{"key":"ref_20","doi-asserted-by":"crossref","first-page":"e02765","DOI":"10.1002\/aenm.202502765","article-title":"A Tough, Adhesive, and Protective Binder Shield for Stabilizing High-Nickel Cathodes in Lithium-Ion Batteries","volume":"15","author":"Jeong","year":"2025","journal-title":"Adv. Energy Mater."},{"key":"ref_21","doi-asserted-by":"crossref","first-page":"151287","DOI":"10.1016\/j.cej.2024.151287","article-title":"Bifunctional Low Molecular Weight Polyacrylic Acid as Aqueous Binder and Coating Agent Enables High Performance LiMn2O4 Cathode for Lithium-Ion Batteries","volume":"489","author":"Shen","year":"2024","journal-title":"Chem. Eng. J."},{"key":"ref_22","doi-asserted-by":"crossref","first-page":"11128","DOI":"10.1021\/acsapm.5c01628","article-title":"Highly Sensitive and Oxidation Resistance Polyacrylic\/Polyacrylamide Hydrogel for Multifunctional Flexible Sensors","volume":"7","author":"Zhang","year":"2025","journal-title":"ACS Appl. Polym. Mater."},{"key":"ref_23","doi-asserted-by":"crossref","first-page":"56910","DOI":"10.1021\/acsami.2c19344","article-title":"Three-Dimensional Crosslinked PAA-TA Hybrid Binders for Long-Cycle-Life SiO\u2093 Anodes in Lithium-Ion Batteries","volume":"14","author":"Tang","year":"2022","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_24","doi-asserted-by":"crossref","first-page":"893","DOI":"10.1016\/j.jcis.2023.12.057","article-title":"Dynamic Hydrogen Bond Cross-Linking Binder with Self-Healing Chemistry Enables High-Performance Silicon Anode in Lithium-Ion Batteries","volume":"657","author":"Chen","year":"2024","journal-title":"J. Colloid Interface Sci."},{"key":"ref_25","doi-asserted-by":"crossref","first-page":"50775","DOI":"10.1021\/acsami.4c10537","article-title":"Chelating Effects of Polyphenolic Biomolecules to Improve \u03b2-MnO2 Cathode Performance for Aqueous Rechargeable Zinc-Ion Batteries","volume":"16","author":"Paik","year":"2024","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_26","doi-asserted-by":"crossref","first-page":"28259","DOI":"10.1038\/s41598-024-80024-x","article-title":"Fabrication of Tannic Acid-Incorporated Polyvinylpyrrolidone\/Polyvinyl Alcohol Composite Hydrogel and Its Application as an Adsorbent for Copper Ion Removal","volume":"14","author":"Chunhakowit","year":"2024","journal-title":"Sci. Rep."},{"key":"ref_27","doi-asserted-by":"crossref","unstructured":"Espina, A., Sanchez-Cortes, S., and Jura\u0161ekov\u00e1, Z. (2022). Vibrational Study (Raman, SERS, and IR) of Plant Gallnut Polyphenols Related to the Fabrication of Iron Gall Inks. Molecules, 27.","DOI":"10.3390\/molecules27010279"},{"key":"ref_28","doi-asserted-by":"crossref","first-page":"e03689","DOI":"10.1002\/adhm.202503689","article-title":"Transparent Multifunctional Wearable Strain Sensor With Self-Healing and Antibacterial Capabilities for Human Motion Detection","volume":"15","author":"Chen","year":"2026","journal-title":"Adv. Healthc. Mater."},{"key":"ref_29","doi-asserted-by":"crossref","first-page":"140038","DOI":"10.1016\/j.electacta.2022.140038","article-title":"Crosslinked Poly(acrylic acid) Enhances Adhesion and Electrochemical Performance of Si Anodes in Li-ion Batteries","volume":"411","author":"He","year":"2022","journal-title":"Electrochim. Acta"},{"key":"ref_30","doi-asserted-by":"crossref","first-page":"1000","DOI":"10.1016\/j.jpowsour.2013.10.039","article-title":"Enabling Aqueous Binders for Lithium Battery Cathodes\u2013Carbon Coating of Aluminum Current Collector","volume":"248","author":"Laszczynski","year":"2014","journal-title":"J. Power Sources"},{"key":"ref_31","doi-asserted-by":"crossref","first-page":"4163","DOI":"10.1021\/acsapm.5c04664","article-title":"Binder Chemistry of Na3 V2 (PO4)2 F3 Cathodes in Aqueous Sodium-Ion Batteries: From \u201cSalt-in-Water\u201d to \u201cWater-in-Salt\u201d","volume":"8","author":"Kareeklin","year":"2026","journal-title":"ACS Appl. Polym. Mater."},{"key":"ref_32","doi-asserted-by":"crossref","first-page":"30302","DOI":"10.1021\/acsami.3c05103","article-title":"Water-soluble polyamide acid binder with fast Li+ transfer kinetics for silicon suboxide anodes in lithium-ion batteries","volume":"15","author":"Li","year":"2023","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"ref_33","doi-asserted-by":"crossref","first-page":"2413865","DOI":"10.1002\/adfm.202413865","article-title":"Stabilizing Nickel-Rich Cathodes in Aqueous Process through Nanocellulose as Water Barrier","volume":"35","author":"Wang","year":"2025","journal-title":"Adv. Funct. Mater."},{"key":"ref_34","doi-asserted-by":"crossref","unstructured":"Neumann, N., Abels, G., Koschek, K., and Boskamp, L. (2023). Crosslinked hyperbranched polyglycerol-based polymer electrolytes for lithium metal batteries. Batteries, 9.","DOI":"10.3390\/batteries9090431"},{"key":"ref_35","doi-asserted-by":"crossref","first-page":"2680","DOI":"10.1021\/acselectrochem.5c00334","article-title":"DRTtools: Freely Accessible Distribution of Relaxation Times Analysis for Electrochemical Impedance Spectroscopy","volume":"1","author":"Wang","year":"2025","journal-title":"ACS Electrochem."},{"key":"ref_36","doi-asserted-by":"crossref","first-page":"2267","DOI":"10.1016\/j.chempr.2023.04.022","article-title":"Charging Processes in Lithium-Oxygen Batteries Unraveled through the Lens of the Distribution of Relaxation Times","volume":"9","author":"Chen","year":"2023","journal-title":"Chem"},{"key":"ref_37","doi-asserted-by":"crossref","first-page":"1172","DOI":"10.1016\/j.joule.2022.05.005","article-title":"The Timescale Identification Decoupling Complicated Kinetic Processes in Lithium Batteries","volume":"6","author":"Lu","year":"2022","journal-title":"Joule"},{"key":"ref_38","doi-asserted-by":"crossref","first-page":"e14492","DOI":"10.1002\/advs.202514492","article-title":"Determination of the Exchange Current Density at Lithium \u2502 Polymer Electrolyte Interfaces","volume":"13","author":"Geng","year":"2026","journal-title":"Adv. Sci."},{"key":"ref_39","doi-asserted-by":"crossref","first-page":"2404652","DOI":"10.1002\/aenm.202404652","article-title":"Unveiling the Mec-based hanism of Mn Dissolution Through a Dynamic Cathode-Electrolyte Interphase on LiMn2O4","volume":"15","author":"Ou","year":"2025","journal-title":"Adv. Energy Mater."},{"key":"ref_40","doi-asserted-by":"crossref","unstructured":"Ciobanu, R., Bucatariu, F., Mihai, M., and Teodosiu, C. (2024). SilicaComposite Sorbents for Heavy Metal Ions Removal from Aqueous Solutions. Polymers, 16.","DOI":"10.3390\/polym16213048"}],"container-title":["Polymers"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.mdpi.com\/2073-4360\/18\/18\/2308\/pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T11:17:03Z","timestamp":1789989423000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.mdpi.com\/2073-4360\/18\/18\/2308"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,9,21]]},"references-count":40,"journal-issue":{"issue":"18","published-online":{"date-parts":[[2026,9]]}},"alternative-id":["polym18182308"],"URL":"https:\/\/doi.org\/10.3390\/polym18182308","relation":{},"ISSN":["2073-4360"],"issn-type":[{"value":"2073-4360","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,9,21]]}}}