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Under light irradiation, Fh can undergo photochemical reactions that influence iron redox cycling and contaminant behavior; however, how Fh formation pH controls its subsequent photochemical reactivity and environmental function remains poorly understood. Herein, Fh was synthesized via the hydrolysis of Fe3+ under pH conditions ranging from 3 to 7 to simulate its formation, and its structural and physicochemical properties (including morphology, crystallinity, and particle size) as well as photochemical activities were then systematically characterized. The results revealed that Fh synthesized under lower pH conditions (e.g., pH \u223c3 in AMD upstream) exhibits low crystallinity and pronounced photoreduction, leading to substantial Fe2+ release, continuous surface renewal, and potential dissolution\u2013precipitation-driven iron redistribution; whereas in neutral downstream environments (pH \u223c7), elevated pH drives the formation of Fh with higher crystallinity, resulting in weakened photoreduction activity, reduced Fe2+ release, and mineral deposition. Importantly, structure\u2013activity fitting revealed that abundant surface Fe\u2013OH govern the photolysis and ligand-to-metal charge transfer (LMCT) activity of Fh, which in turn influences \u2022OH generation. These results indicate that Fh in AMD systems functions not as a passively aging mineral particle, but as a dynamically renewed photoreactive phase whose redox activity, aging behavior, and phase transformation are preconditioned by Fh formation pH. This study provides novel insights into the spatial variability of iron mobility and contaminant fate in AMD systems, with implications for predictive modeling and remediation strategies.<\/jats:p>","DOI":"10.1021\/acs.est.6c01785","type":"journal-article","created":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T12:27:12Z","timestamp":1784118432000},"page":"20361-20371","source":"Crossref","is-referenced-by-count":0,"title":["Effect of Formation\npH on the Structure of Ferrihydrite\nand Its Photochemical Activity"],"prefix":"10.1021","volume":"60","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9638-3760","authenticated-orcid":true,"given":"Ying","family":"Lv","sequence":"first","affiliation":[{"name":"Shaoxing University , , Huancheng West Road 508 , , ,","place":["Shaoxing, China, 312000"]},{"name":"Chinese Academy of Sciences , , ,","place":["Guangzhou, China, 510640"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0876-4094","authenticated-orcid":true,"given":"Jianfa","family":"Li","sequence":"additional","affiliation":[{"name":"Shaoxing University , , Huancheng West Road 508 , , ,","place":["Shaoxing, China, 312000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qing","family":"Liao","sequence":"additional","affiliation":[{"name":"Shaoxing University , , Huancheng West Road 508 , , ,","place":["Shaoxing, China, 312000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yixuan","family":"Yang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Guangzhou, China, 510640"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiangang","family":"Hu","sequence":"additional","affiliation":[{"name":"National Center for Quality Inspection and Testing of Chinese Rice Wine , , ,","place":["Shaoxing, China, 312000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yimin","family":"Li","sequence":"additional","affiliation":[{"name":"Shaoxing University , , Huancheng West Road 508 , , ,","place":["Shaoxing, China, 312000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huaping","family":"Dong","sequence":"additional","affiliation":[{"name":"Shaoxing University , , Huancheng West Road 508 , , ,","place":["Shaoxing, China, 312000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7591-6625","authenticated-orcid":true,"given":"Runliang","family":"Zhu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Guangzhou, China, 510640"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,15]]},"reference":[{"key":"2026072809081918100_cit1","doi-asserted-by":"publisher","first-page":"100024","DOI":"10.1016\/j.ese.2020.100024","article-title":"Biological remediation of acid mine drainage: Review\nof past trends and current outlook","volume":"2","author":"Rambabu","year":"2020","journal-title":"Env. 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Technol."},{"key":"2026072809081918100_cit5","doi-asserted-by":"publisher","first-page":"811","DOI":"10.1021\/acsearthspacechem.1c00334","article-title":"Photoreductive dissolution\nof iron (hydr)oxides and its geochemical\nsignificance","volume":"6","author":"Lv","year":"2022","journal-title":"ACS Earth Space Chem."},{"key":"2026072809081918100_cit6","doi-asserted-by":"publisher","first-page":"155835","DOI":"10.1016\/j.scitotenv.2022.155835","article-title":"Enhanced immobilization\nof phosphate by ferrihydrite\nduring the photoreductive dissolution process","volume":"838","author":"Lv","year":"2022","journal-title":"Sci. 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Colloid Interface Sci."},{"issue":"2\u20133","key":"2026072809081918100_cit21","doi-asserted-by":"publisher","first-page":"210","DOI":"10.1016\/j.crte.2010.11.001","article-title":"Composition and\nstructural aspects\nof naturally occurring ferrihydrite","volume":"343","author":"Cismasu","year":"2011","journal-title":"C.R. Geosci."},{"issue":"46","key":"2026072809081918100_cit22","doi-asserted-by":"publisher","first-page":"20480","DOI":"10.1021\/acs.est.4c06885","article-title":"Deciphering\nthe roles\nof molecular weight and carboxyl richness of organic matter on their\nadsorption onto ferrihydrite nanoparticles and the resulting aggregation","volume":"58","author":"Li","year":"2024","journal-title":"Environ. Sci. Technol."},{"issue":"13","key":"2026072809081918100_cit23","doi-asserted-by":"publisher","first-page":"3249","DOI":"10.1016\/j.gca.2005.01.023","article-title":"Electronic\nstructures of iron(III) and manganese(IV) (hydr)oxide minerals: Thermodynamics\nof photochemical reductive dissolution in aquatic environments","volume":"69","author":"Sherman","year":"2005","journal-title":"Geochim. Cosmochim. 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Technol."},{"issue":"13","key":"2026072809081918100_cit26","doi-asserted-by":"publisher","first-page":"135703","DOI":"10.1088\/0957-4484\/25\/13\/135703","article-title":"Sensitive detection\nof surface- and size-dependent direct and indirect band gap transitions\nin ferritin","volume":"25","author":"Colton","year":"2014","journal-title":"Nanotechnology"},{"issue":"1","key":"2026072809081918100_cit27","doi-asserted-by":"publisher","first-page":"12609","DOI":"10.1038\/s41598-017-12791-9","article-title":"Formation of iron oxide nanoparticles\nfor the photooxidation of water: Alteration of finite size effects\nfrom ferrihydrite to hematite","volume":"7","author":"Schwaminger","year":"2017","journal-title":"Sci. Rep."},{"issue":"1","key":"2026072809081918100_cit28","doi-asserted-by":"publisher","first-page":"190","DOI":"10.1039\/C5EN00191A","article-title":"Effects\nof crystallite size on the structure and magnetism of ferrihydrite","volume":"3","author":"Wang","year":"2016","journal-title":"Environ. Sci.: Nano"},{"issue":"12","key":"2026072809081918100_cit29","doi-asserted-by":"publisher","first-page":"7309","DOI":"10.1021\/acs.est.0c00996","article-title":"Citrate controls\nFe(II)-catalyzed transformation of ferrihydrite by complexation of\nthe labile Fe(III) intermediate","volume":"54","author":"Sheng","year":"2020","journal-title":"Environ. Sci.\nTechnol."},{"issue":"15","key":"2026072809081918100_cit30","doi-asserted-by":"publisher","first-page":"8854","DOI":"10.1021\/acs.est.9b02750","article-title":"Solar irradiation induced transformation\nof ferrihydrite in the presence of aqueous Fe2+","volume":"53","author":"Shu","year":"2019","journal-title":"Environ. Sci. Technol."},{"issue":"32","key":"2026072809081918100_cit31","doi-asserted-by":"publisher","first-page":"14467","DOI":"10.1021\/acs.jpcc.5c03617","article-title":"Improving nanoparticles structural analysis by pair\ndistribution function from electron diffraction","volume":"129","author":"Mogili","year":"2025","journal-title":"J. Phys. Chem. C"},{"issue":"3","key":"2026072809081918100_cit32","doi-asserted-by":"publisher","first-page":"47","DOI":"10.1186\/1467-4866-6-47","article-title":"Quantifying hydrogen peroxide in\niron-containing solutions using leuco crystal violet","volume":"6","author":"Cohn","year":"2005","journal-title":"Geochem. Trans."},{"issue":"9","key":"2026072809081918100_cit33","doi-asserted-by":"publisher","first-page":"3966","DOI":"10.1039\/D3EN00930K","article-title":"Formation\nand transformation of iron oxy-hydroxide precursor clusters to ferrihydrite","volume":"11","author":"Namayandeh","year":"2024","journal-title":"Environ. Sci.: Nano"},{"issue":"4","key":"2026072809081918100_cit34","doi-asserted-by":"publisher","first-page":"1682","DOI":"10.1039\/d3en00828b","article-title":"Influence\nof time and ageing conditions on the properties of ferrihydrite","volume":"11","author":"Sassi","year":"2024","journal-title":"Environ. Sci.: Nano"},{"issue":"11","key":"2026072809081918100_cit35","doi-asserted-by":"publisher","first-page":"987","DOI":"10.1130\/g45386.1","article-title":"A new model\nfor transformation of ferrihydrite to hematite in soils and sediments","volume":"46","author":"Jiang","year":"2018","journal-title":"Geology"},{"key":"2026072809081918100_cit36","doi-asserted-by":"publisher","first-page":"552","DOI":"10.1016\/j.envres.2019.03.008","article-title":"Aggregation of ferrihydrite nanoparticles: effects of pH, electrolytes,\nand organics","volume":"172","author":"Liu","year":"2019","journal-title":"Environ. 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Rep."},{"issue":"6","key":"2026072809081918100_cit38","doi-asserted-by":"publisher","first-page":"737","DOI":"10.1346\/CCMN.1994.0420610","article-title":"Ferrihydrite: Surface\nstructure and its effects on phase transformation","volume":"42","author":"Zhao","year":"1994","journal-title":"Clays Clay Miner"},{"issue":"2","key":"2026072809081918100_cit39","doi-asserted-by":"publisher","first-page":"185","DOI":"10.1180\/claymin.1993.028.2.02","article-title":"Structural model for\nferrihydrite","volume":"28","author":"Drits","year":"1993","journal-title":"Clay Miner."},{"issue":"1","key":"2026072809081918100_cit40","doi-asserted-by":"publisher","first-page":"79","DOI":"10.1038\/s42004-020-0325-y","article-title":"Direct identification\nof reaction sites on ferrihydrite","volume":"3","author":"Boily","year":"2020","journal-title":"Commun. Chem."},{"issue":"8","key":"2026072809081918100_cit41","doi-asserted-by":"publisher","first-page":"2579","DOI":"10.1039\/c2cp22715k","article-title":"Structural controls\non OH site availability and reactivity\nat iron oxyhydroxide particle surfaces","volume":"14","author":"Song","year":"2012","journal-title":"Phys.\nChem. Chem. Phys."},{"issue":"10","key":"2026072809081918100_cit42","doi-asserted-by":"publisher","first-page":"2251","DOI":"10.1016\/0016-7037(93)90567-G","article-title":"Surface chemistry\nof ferrihydrite: Part 1. EXAFS studies of the geometry of coprecipitated\nand adsorbed arsenate","volume":"57","author":"Waychunas","year":"1993","journal-title":"Geochim. Cosmochim. Acta"},{"issue":"15","key":"2026072809081918100_cit43","doi-asserted-by":"publisher","first-page":"4423","DOI":"10.1016\/j.gca.2009.04.032","article-title":"A surface structural model for ferrihydrite I: Sites\nrelated to primary charge, molar mass, and mass density","volume":"73","author":"Hiemstra","year":"2009","journal-title":"Geochim. Cosmochim. Acta"},{"key":"2026072809081918100_cit44","doi-asserted-by":"publisher","first-page":"125002","DOI":"10.1016\/j.apcatb.2024.125002","article-title":"Fe(III) alleviates\npH dependence of iron-based bimetallic\/PMS system\nfor organic pollutant oxidation","volume":"366","author":"Yuan","year":"2025","journal-title":"Appl. Catal.,\nB"},{"issue":"31","key":"2026072809081918100_cit45","doi-asserted-by":"publisher","first-page":"13263","DOI":"10.1021\/jp953650b","article-title":"Electronic\nstructure and properties of solids","volume":"100","author":"Burdett","year":"1996","journal-title":"J. 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