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Herein, we confine highly dispersed iodine quantum dots within a Fe(CN)64\u2013-doped polypyrrole\/polyaniline framework to establish a free-energy-gradient-driven regeneration pathway. During discharge, Fe-cyanide and N-rich sites immobilize polyiodide intermediates, suppressing shuttle and self-discharge. More importantly, during charging, the in situ generated ZnxFeIII(CN)6\/Znx+1FeII(CN)6 redox couple establishes an intrinsic free-energy gradient that couples Zn2+ transfer with iodide oxidation, thereby directing iodine regeneration and limiting aggregation. The resulting cathode delivers 238.2 mAh g\u20131 at 0.5 A g\u20131, maintains approximately 217 mAh g\u20131 at 10 A g\u20131, retains 92.6% capacity after 50,000 cycles with nearly 100% Coulombic efficiency, and supports stable pouch-cell and flexible microbattery operation. These results establish free-energy-gradient engineering as a strategy for regulating reversible halogen conversion beyond static confinement.<\/jats:p>","DOI":"10.1021\/acs.nanolett.6c03332","type":"journal-article","created":{"date-parts":[[2026,8,22]],"date-time":"2026-08-22T00:38:43Z","timestamp":1787359123000},"page":"11573-11582","source":"Crossref","is-referenced-by-count":0,"title":["Free-Energy-Gradient-Driven\nIodine Regeneration toward\nUltrastable Zinc\u2013Iodine Batteries"],"prefix":"10.1021","volume":"26","author":[{"given":"Zhibo","family":"Zhang","sequence":"first","affiliation":[{"name":"Jilin University , , , ,","place":["Changchun, Jilin, China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaofan","family":"Liu","sequence":"additional","affiliation":[{"name":"Jilin University , , , ,","place":["Changchun, Jilin, China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Runze","family":"Xia","sequence":"additional","affiliation":[{"name":"Jilin University , , , ,","place":["Changchun, Jilin, China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0004-6174-6364","authenticated-orcid":true,"given":"Hong","family":"Zhang","sequence":"additional","affiliation":[{"name":"Jilin University , , , ,","place":["Changchun, Jilin, China, 130022"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8086-9686","authenticated-orcid":true,"given":"Ke","family":"Lu","sequence":"additional","affiliation":[{"name":"Jilin University , , , ,","place":["Changchun, Jilin, China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6413-0689","authenticated-orcid":true,"given":"Fei","family":"Du","sequence":"additional","affiliation":[{"name":"Jilin University , , , ,","place":["Changchun, Jilin, China, 130012"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,21]]},"reference":[{"issue":"9","key":"2026090311585752900_cit1","doi-asserted-by":"publisher","first-page":"3071","DOI":"10.1039\/D3SC06150G","article-title":"Advancements in Aqueous Zinc-Iodine\nBatteries: A Review","volume":"15","author":"Bai","year":"2024","journal-title":"Chem. 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Energy Mater."},{"issue":"7","key":"2026090311585752900_cit32","doi-asserted-by":"publisher","first-page":"3160","DOI":"10.1039\/D5EE00027K","article-title":"Dual-Plating Aqueous\nZn-Iodine Batteries Enabled via Halogen-Complexation Chemistry for\nLarge-Scale Energy Storage","volume":"18","author":"Li","year":"2025","journal-title":"Energy Environ.\nSci."},{"issue":"8","key":"2026090311585752900_cit33","doi-asserted-by":"publisher","first-page":"2723","DOI":"10.1039\/D6EE00296J","article-title":"Separator-Free Aqueous Zinc-Iodine Batteries: An in\nsitu Dual-Confinement Interface Enabling Electrostatic Reversible\nPolyiodide Capture\/Release","volume":"19","author":"Liu","year":"2026","journal-title":"Energy Environ.\nSci."},{"issue":"14","key":"2026090311585752900_cit34","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202521374","article-title":"Supramolecularly Engineered Flexible Zinc-Iodine Batteries\nfor Wearable Electronics","volume":"38","author":"Huang","year":"2026","journal-title":"Adv. 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Commun."},{"issue":"1","key":"2026090311585752900_cit39","doi-asserted-by":"publisher","first-page":"3048","DOI":"10.1038\/s41467-026-69743-z","article-title":"Carbon-Halogen\nBond Substitution Enables High-Utilization\nFour-Electron Iodine Redox in Noncorrosive Dilute Electrolytes","volume":"17","author":"Shi","year":"2026","journal-title":"Nat. Commun."},{"issue":"4","key":"2026090311585752900_cit40","doi-asserted-by":"publisher","first-page":"1266","DOI":"10.1039\/D5EE07366A","article-title":"Fused-Ring Topology Orchestrates\nCrystallographic Control and Polyiodide Sequestration for Ultra-Durable\nZinc-Iodine Batteries","volume":"19","author":"Jin","year":"2026","journal-title":"Energy Environ. Sci."},{"issue":"26","key":"2026090311585752900_cit41","doi-asserted-by":"publisher","first-page":"27858","DOI":"10.1021\/jacs.6c09194","article-title":"Dynamic\nAdaptive Interfaces Enable Zn-Iodine Hydrogel Batteries with High\nAreal Capacity and Low Self-Discharge","volume":"148","author":"Cai","year":"2026","journal-title":"J. Am.\nChem. Soc."},{"issue":"4","key":"2026090311585752900_cit42","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202515756","article-title":"A Diffusion-Retarded Strategy for Practical Zn-I2 Batteries Under Harsh Conditions","volume":"65","author":"Lian","year":"2026","journal-title":"Angew.\nChem., Int. 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