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During the oxidation of phenolic contaminants, however, soluble coupling products and Mn-containing species (e.g., MnOx colloids and dissolved Mn ions) may remain in the aqueous phase, increasing the burden of downstream separation. Herein, we demonstrate that commercial polyferric sulfate (PFS) can simultaneously serve as a KMnO4 activator and an in situ coagulant, establishing a one-step synergistic polymerization-coagulation strategy for efficient 4-chlorophenol (4-CP) removal with minimal soluble oligomers and leachable metal species. Mechanistic studies reveal that PFS forms a positively charged Fe-(hydr)oxide interface that facilitates KMnO4 activation via electrostatic interactions. Meanwhile, PFS serves as a solid scaffold that stabilizes the critical 4-chlorophenoxyl radical intermediate via bis(4-chlorocatecholato)iron(III) complex formation, thereby driving polymer chain growth. Leveraging its inherent coagulation property, PFS effectively captures organic polymers, increasing chemical oxygen demand (COD) removal from 35.4% to 56.2% within 10 min, while efficiently sequestering MnOx colloids and reducing residual Fe and Mn concentrations in the treated supernatant by 99.2% and 99.4%, respectively. This work addresses limitations of conventional KMnO4 oxidation through in situ polymerization-coagulation, offering a strategy for phenolic pollutant remediation with reduced soluble oligomer accumulation and metal residuals.<\/jats:p>","DOI":"10.1021\/acs.est.6c12061","type":"journal-article","created":{"date-parts":[[2026,9,2]],"date-time":"2026-09-02T12:07:10Z","timestamp":1788350830000},"page":"25935-25946","source":"Crossref","is-referenced-by-count":1,"title":["Achieving Polymerization-Oriented\nPhenolic Pollutant\nCapture and Minimized Metal Residue in the Permanganate\/Polyferric\nSulfate Process via a Synergistic Polymerization-Coagulation Strategy"],"prefix":"10.1021","volume":"60","author":[{"given":"Bingyuan","family":"Xu","sequence":"first","affiliation":[{"name":"Huazhong University of Science and Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lixin","family":"Tian","sequence":"additional","affiliation":[{"name":"Huazhong University of Science and Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dong","family":"Xu","sequence":"additional","affiliation":[{"name":"Hubei Provincial Academy of Eco-Environmental Sciences , ,","place":["Wuhan, China, 430074"]},{"name":"Wuhan University , , ,","place":["Wuhan, China, 430072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7243-0806","authenticated-orcid":true,"given":"Jing","family":"Chen","sequence":"additional","affiliation":[{"name":"Huazhong University of Science and Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaohui","family":"Wu","sequence":"additional","affiliation":[{"name":"Huazhong University of Science and Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2278-3299","authenticated-orcid":true,"given":"Tao","family":"Zhou","sequence":"additional","affiliation":[{"name":"Huazhong University of Science and Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6054-3021","authenticated-orcid":true,"given":"Mingjie","family":"Huang","sequence":"additional","affiliation":[{"name":"Huazhong University of Science and Technology , , ,","place":["Wuhan, China, 430074"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,29]]},"reference":[{"key":"2026091511114037700_cit1","doi-asserted-by":"publisher","first-page":"131746","DOI":"10.1016\/j.jhazmat.2023.131746","article-title":"Permanganate activation\nwith Mn oxides at different oxidation states: Insight into the surface-promoted\nelectron transfer mechanism","volume":"457","author":"Ma","year":"2023","journal-title":"J. Hazard. Mater."},{"key":"2026091511114037700_cit2","doi-asserted-by":"publisher","first-page":"117513","DOI":"10.1016\/j.watres.2021.117513","article-title":"Oxidative transformation\nof emerging organic contaminants by aqueous permanganate: Kinetics,\nproducts, toxicity changes, and effects of manganese products","volume":"203","author":"Li","year":"2021","journal-title":"Water Res."},{"key":"2026091511114037700_cit3","doi-asserted-by":"publisher","first-page":"119265","DOI":"10.1016\/j.watres.2022.119265","article-title":"Enhanced oxidation\nof organic contaminants by Mn(VII). in water","volume":"226","author":"Guan","year":"2022","journal-title":"Water Res."},{"key":"2026091511114037700_cit4","doi-asserted-by":"publisher","first-page":"100421","DOI":"10.1016\/j.ese.2024.100421","article-title":"Overlooked\ninteraction between redox-mediator\nand bisphenol-A in permanganate oxidation","volume":"21","author":"Zhang","year":"2024","journal-title":"Environ.\nSci. Ecotechnology"},{"key":"2026091511114037700_cit5","doi-asserted-by":"publisher","first-page":"123784","DOI":"10.1016\/j.watres.2025.123784","article-title":"Coexisting\nAnilines Accelerate the Oxidation of Phenolics by Manganese Oxides","volume":"283","author":"Cui","year":"2025","journal-title":"Water Res."},{"key":"2026091511114037700_cit6","doi-asserted-by":"publisher","first-page":"164920","DOI":"10.1016\/j.cej.2025.164920","article-title":"High efficiency phenol removal from\nwastewater with low energy consumption enabled by an electropolymerization\nmembrane reactor","volume":"519","author":"Wang","year":"2025","journal-title":"Chem. Eng. 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Sustainable"},{"key":"2026091511114037700_cit9","doi-asserted-by":"publisher","first-page":"48","DOI":"10.1016\/j.seppur.2013.01.023","article-title":"Oxidative\nremoval of bisphenol A by permanganate: Kinetics,\npathways and influences of co-existing chemicals","volume":"107","author":"Zhang","year":"2013","journal-title":"Sep. Purif. 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Sci.:\nProcesses Impacts"},{"issue":"44","key":"2026091511114037700_cit22","doi-asserted-by":"publisher","first-page":"19851","DOI":"10.1021\/acs.est.4c06818","article-title":"Speciation Controls\nthe Kinetics of Iron Hydroxide Precipitation and Transformation at\nAlkaline pH","volume":"58","author":"Furcas","year":"2024","journal-title":"Environ. Sci. Technol."},{"issue":"3","key":"2026091511114037700_cit23","doi-asserted-by":"publisher","first-page":"339","DOI":"10.1039\/C6EM00694A","article-title":"Oxidation potentials of phenols and\nanilines: correlation analysis of electrochemical and theoretical\nvalues","volume":"19","author":"Pavitt","year":"2017","journal-title":"Environ. Sci.: Processes Impacts"},{"issue":"8","key":"2026091511114037700_cit24","doi-asserted-by":"publisher","first-page":"4728","DOI":"10.1021\/acs.est.1c03621","article-title":"Permanganate Oxidation of Organic\nContaminants and Model Compounds","volume":"56","author":"Laszakovits","year":"2022","journal-title":"Environ. Sci.\nTechnol."},{"key":"2026091511114037700_cit25","doi-asserted-by":"publisher","first-page":"164086","DOI":"10.1016\/j.scitotenv.2023.164086","article-title":"Influence and mechanism of water matrices on H2O2-based Fenton-like oxidation processes: A review","volume":"888","author":"Cheng","year":"2023","journal-title":"Sci. Total Environ."},{"issue":"1","key":"2026091511114037700_cit26","doi-asserted-by":"publisher","first-page":"129","DOI":"10.1021\/acsearthspacechem.8b00160","article-title":"Carbonate adsorption to ferrihydrite: Competitive interaction\nwith phosphate for use in soil systems","volume":"3","author":"Mendez","year":"2019","journal-title":"ACS\nEarth Space Chem."},{"issue":"19","key":"2026091511114037700_cit27","doi-asserted-by":"publisher","first-page":"8576","DOI":"10.1021\/acs.est.4c00988","article-title":"Unraveling the Role of Humic Acid\nin the Oxidation of Phenolic Contaminants\nby Soluble Manganese Oxo-Anions","volume":"58","author":"Wang","year":"2024","journal-title":"Environ. Sci.\nTechnol."},{"key":"2026091511114037700_cit28","doi-asserted-by":"publisher","first-page":"121170","DOI":"10.1016\/j.watres.2024.121170","article-title":"Enhanced permanganate\noxidation of phenolic pollutants by alumina and potential industrial\napplication","volume":"251","author":"Zhang","year":"2024","journal-title":"Water Res."},{"key":"2026091511114037700_cit29","doi-asserted-by":"publisher","first-page":"136678","DOI":"10.1016\/j.jhazmat.2024.136678","article-title":"Phenols coupled\nduring oxidation upstream of water treatment would generate higher\ntoxic coupling phenolic disinfection by-products during chlorination\ndisinfection","volume":"483","author":"Gao","year":"2025","journal-title":"J. Hazard. Mater."},{"issue":"1","key":"2026091511114037700_cit30","doi-asserted-by":"publisher","first-page":"2327","DOI":"10.1038\/s41467-024-46739-1","article-title":"Tailoring d-band\ncenter of high-valent metal-oxo species for pollutant removal via\ncomplete polymerization","volume":"15","author":"Liu","year":"2024","journal-title":"Nat. Commun."},{"key":"2026091511114037700_cit31","doi-asserted-by":"publisher","first-page":"119200","DOI":"10.1016\/j.watres.2022.119200","article-title":"Enhanced coagulation\nand oxidation by the Mn(VII)-Fe(III)\/peroxymonosulfate process: Performance\nand mechanisms","volume":"226","author":"Dong","year":"2022","journal-title":"Water Res."},{"key":"2026091511114037700_cit32","doi-asserted-by":"publisher","first-page":"121894","DOI":"10.1016\/j.susc.2021.121894","article-title":"On the wrong\nassignment of the XPS O1s signal at 531\u2013532 eV attributed to\noxygen vacancies in photo- and electro-catalysts for water splitting\nand other materials applications","volume":"712","author":"Idriss","year":"2021","journal-title":"Surf. Sci."},{"issue":"14","key":"2026091511114037700_cit33","doi-asserted-by":"publisher","first-page":"5902","DOI":"10.1021\/ac900621f","article-title":"Martin\u2019s\nRule for High-Performance Liquid Chromatography\nRetention of Polystyrene Oligomers","volume":"81","author":"Kim","year":"2009","journal-title":"Anal. Chem."},{"key":"2026091511114037700_cit34","doi-asserted-by":"publisher","first-page":"124863","DOI":"10.1016\/j.watres.2025.124863","article-title":"New insights\ninto the process of phenolic degradation by high-valent iron - a proton-coupled\nelectron process","volume":"289","author":"Lin","year":"2026","journal-title":"Water Res."},{"issue":"14","key":"2026091511114037700_cit35","doi-asserted-by":"publisher","first-page":"3371","DOI":"10.1021\/ja002453+","article-title":"Construction\nof Persistent Phenoxyl Radical with Intramolecular Hydrogen Bonding","volume":"123","author":"Maki","year":"2001","journal-title":"J. Am. Chem. 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Acta"},{"key":"2026091511114037700_cit40","doi-asserted-by":"publisher","first-page":"118528","DOI":"10.1016\/j.watres.2022.118528","article-title":"Enhanced\ndegradation of emerging contaminants by permanganate\/quinone process:\nCase study with bisphenol A","volume":"219","author":"Dong","year":"2022","journal-title":"Water Res."},{"key":"2026091511114037700_cit41","doi-asserted-by":"publisher","first-page":"123069","DOI":"10.1016\/j.watres.2024.123069","article-title":"New insight\ninto enhanced permanganate oxidation by lignocellulose-derived biochar:\nThe overlooked role of persistent free radicals","volume":"274","author":"Tian","year":"2025","journal-title":"Water Res."},{"issue":"40","key":"2026091511114037700_cit42","doi-asserted-by":"publisher","first-page":"18041","DOI":"10.1021\/acs.est.4c06557","article-title":"Proton vs Electron:\nThe Dual Role of Redox-Inactive Metal Ions in\nPermanganate Oxidation Kinetics","volume":"58","author":"Luo","year":"2024","journal-title":"Environ. Sci.\nTechnol."},{"issue":"6","key":"2026091511114037700_cit43","doi-asserted-by":"publisher","first-page":"718","DOI":"10.1134\/S1061934823040093","article-title":"Determination of Lignin, Cellulose,\nand Hemicellulose in Plant Materials by FTIR Spectroscopy","volume":"78","author":"Kostryukov","year":"2023","journal-title":"J. Anal. Chem."},{"issue":"19","key":"2026091511114037700_cit44","doi-asserted-by":"publisher","first-page":"7423","DOI":"10.1021\/es901346z","article-title":"Surface Complexation\nof Carboxylate Adheres Cryptosporidium parvum O\u0308ocysts to the\nHematite-Water Interface","volume":"43","author":"Gao","year":"2009","journal-title":"Environ. Sci. Technol."},{"issue":"4","key":"2026091511114037700_cit45","doi-asserted-by":"publisher","first-page":"441","DOI":"10.1002\/etc.5620100403","article-title":"Adsorption\nof phenol and substituted phenols by iron\noxides","volume":"10","author":"McBride","year":"1991","journal-title":"Environ. Toxicol. Chem."},{"key":"2026091511114037700_cit46","doi-asserted-by":"publisher","first-page":"337","DOI":"10.1016\/j.apsusc.2017.02.002","article-title":"X-Ray Photoelectron\nSpectroscopic Characterization of Iron Oxide Nanoparticles","volume":"405","author":"Radu","year":"2017","journal-title":"Appl. Surf. Sci."},{"key":"2026091511114037700_cit47","doi-asserted-by":"publisher","first-page":"120562","DOI":"10.1016\/j.watres.2023.120562","article-title":"Enhancing\nthe Abatement of Permanganate-inert Micropollutants: Multiple Roles\nof Nascent Manganese Dioxide in Permanganate Oxidation","volume":"245","author":"Wu","year":"2023","journal-title":"Water Res."},{"issue":"11","key":"2026091511114037700_cit48","doi-asserted-by":"publisher","first-page":"2687","DOI":"10.1021\/acsestengg.4c00333","article-title":"Iron Enhancing\nSuperoxide-Mediated Mn(II). Oxidation by Peroxymonosulfate: Elucidating\nthe Role of Superoxide Radicals","volume":"4","author":"Hua","year":"2024","journal-title":"ACS EST Eng."},{"issue":"30","key":"2026091511114037700_cit49","doi-asserted-by":"publisher","first-page":"16001","DOI":"10.1021\/acs.est.5c02183","article-title":"Efficient\nPolymerization Removal of Phenolic Pollutants by In Situ-Formed Iron-Complexes\nin Thermally Activated Peroxydisulfate Systems","volume":"59","author":"Li","year":"2025","journal-title":"Environ. Sci. Technol."},{"key":"2026091511114037700_cit50","doi-asserted-by":"publisher","first-page":"125930","DOI":"10.1016\/j.jhazmat.2021.125930","article-title":"Simultaneous\nadsorption of Cr(VI). and phenol by biochar-based iron\noxide composites in water: Performance, kinetics and mechanism","volume":"416","author":"Dong","year":"2021","journal-title":"J. Hazard. Mater."},{"issue":"20","key":"2026091511114037700_cit51","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2302407120","article-title":"Distinguishing homogeneous advanced oxidation processes\nin bulk water from heterogeneous surface reactions in organic oxidation","volume":"120","author":"Zhang","year":"2023","journal-title":"Proc. Natl. Acad. Sci. U. S. A."},{"issue":"12","key":"2026091511114037700_cit52","doi-asserted-by":"publisher","first-page":"9672","DOI":"10.1021\/acs.est.5c17609","article-title":"Unexpected Polymerization Pathway in the Carbocatalysts\/Permanganate\nProcesses for Water Decontamination","volume":"60","author":"Zhou","year":"2026","journal-title":"Environ.\nSci. 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