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Unlike conventional Super P (SP):PVDF systems, P3HT can be electrochemically doped within the LFP operating potential range, forming an internal percolating conductive network that precedes and facilitates the LFP redox reaction. Strong \u03c0\u2013\u03c0 interactions and P3HT\u2013Fe coordination enable P3HT to uniformly coat LFP particles, yielding intimate interfacial contact, enhanced adhesion, and an ultrathin, stable cathode\u2013electrolyte interphase. As a result, P3HT\u2010based LFP cathodes exhibit significantly improved packing density (2.70 g cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    ), delivering volumetric energy densities up to 1402 Wh L\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    , far surpassing SP:PVDF\u2010based counterparts (1.43 g cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    ; 738 Wh L\n                    <jats:sup>\u22121<\/jats:sup>\n                    ). The P3HT\u2010based LFP cathodes achieve long\u2010term cycling stability and high\u2010rate capability comparable to or better than SP:PVDF\u2010based LFP electrodes. Density functional theory further reveals strong P3HT\u2013LFP adsorption (\u221280 to \u2212170 kJ mol\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    ), substantial charge transfer, and narrowed bandgap at the P3HT\u2010LFP interface, confirming enhanced electronic coupling. This work shows that P3HT as a highly efficient binder can integrate conductivity, redox mediation, and interfacial stabilization, offering a compelling strategy for constructing next\u2010generation high\u2010density, long\u2010life LFP cathodes.\n                  <\/jats:p>","DOI":"10.1002\/smll.76059","type":"journal-article","created":{"date-parts":[[2026,10,4]],"date-time":"2026-10-04T13:05:20Z","timestamp":1791119120000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Pristine Poly(3\u2010hexylthiophene) as an On\u2010Demand Conductive Binder and Redox Mediator for Carbon\u2010Additive\u2010Free, High\u2010Volumetric\u2010Energy\u2010Density, LiFePO\n                    <sub>4<\/sub>\n                    Cathodes without 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Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3679-8133","authenticated-orcid":false,"given":"Yuning","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering and Waterloo Institute for Nanotechnology (WIN) University of Waterloo  Waterloo Ontario 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