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However, the key DOM components and their molecular transformations associated with this electron-transfer process remain poorly resolved. Here, by integrating Fourier transform ion cyclotron resonance mass spectrometry with machine learning, we reveal that fulvic acid (FA), the predominant DOM fraction, undergoes selective molecular transformation by Geobacter sulfurreducens PCA, forming a reactive subpool that drives O2 activation and thereby enhances As(III) oxidation by approximately 2\u201310 fold. Reaction network analysis reveals that oxygen-rich aromatic precursors are preferentially transformed into more reduced intermediates through decarboxylation, dehydrogenation, and partial reduction pathways. These transformations collectively shift the molecular composition toward lower oxidation states and enhanced redox reactivity. Machine-learning analysis further identifies nitrogen- and sulfur-containing molecules with low oxidation states as the key components governing the overall redox activity of the system. These species represent a functionally distinct fraction of microbially transformed FA with enhanced electron-donating capacity. This study provides molecular-level insights into how microbial DOM transformation regulates O2 activation and As(III) oxidation, offering a mechanistic basis for predicting and manipulating redox reactivity in dynamic soil and sediment systems.<\/jats:p>","DOI":"10.1021\/acs.est.6c05728","type":"journal-article","created":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T15:01:47Z","timestamp":1786978907000},"page":"27818-27828","source":"Crossref","is-referenced-by-count":0,"title":["Microbial Reduction\u2013Induced\nSelective DOM Transformation\nGoverns As(III) Oxidation under Redox Oscillations"],"prefix":"10.1021","volume":"60","author":[{"given":"Xiangjun","family":"Meng","sequence":"first","affiliation":[{"name":"Henan Normal University , , , , ,","place":["Xinxiang, Henan, PR China, 453007"]},{"name":"Guangdong Academy of Sciences , , ,","place":["Guangzhou, China, 510650"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7312-9524","authenticated-orcid":true,"given":"Jialin","family":"Chi","sequence":"additional","affiliation":[{"name":"Guangdong Academy of Sciences , , ,","place":["Guangzhou, China, 510650"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mengmeng","family":"Yin","sequence":"additional","affiliation":[{"name":"Henan Normal University , , , , ,","place":["Xinxiang, Henan, PR China, 453007"]},{"name":"Guangdong Academy of Sciences , , ,","place":["Guangzhou, China, 510650"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4220-3098","authenticated-orcid":true,"given":"Shiyin","family":"Wu","sequence":"additional","affiliation":[{"name":"Guangdong Academy of Sciences , , ,","place":["Guangzhou, China, 510650"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kai","family":"Liu","sequence":"additional","affiliation":[{"name":"Guangdong Academy of Sciences , , ,","place":["Guangzhou, China, 510650"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin","family":"Zhang","sequence":"additional","affiliation":[{"name":"Henan Normal University , , , , ,","place":["Xinxiang, Henan, PR China, 453007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kai","family":"Jiang","sequence":"additional","affiliation":[{"name":"Henan Normal University , , , , ,","place":["Xinxiang, Henan, PR China, 453007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Christine V.","family":"Putnis","sequence":"additional","affiliation":[{"name":"University of Mu\u0308nster , , ,","place":["Mu\u0308nster, Germany, 48149"]},{"name":"Curtin University , , ,","place":["Perth, Australia, 6845"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6508-8750","authenticated-orcid":true,"given":"Xiaoxia","family":"Zhou","sequence":"additional","affiliation":[{"name":"Guangdong Academy of Sciences , , ,","place":["Guangzhou, China, 510650"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4609-1190","authenticated-orcid":true,"given":"Liping","family":"Fang","sequence":"additional","affiliation":[{"name":"Guangdong Academy of Sciences , , ,","place":["Guangzhou, China, 510650"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9027-9313","authenticated-orcid":true,"given":"Fangbai","family":"Li","sequence":"additional","affiliation":[{"name":"Guangdong Academy of Sciences , , ,","place":["Guangzhou, China, 510650"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,17]]},"reference":[{"issue":"9","key":"2026100609064164700_cit1","doi-asserted-by":"publisher","first-page":"659","DOI":"10.1038\/s43017-023-00470-5","article-title":"Coupled iron cycling and organic matter transformation\nacross redox interfaces","volume":"4","author":"Dong","year":"2023","journal-title":"Nat. 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Mater."},{"issue":"1","key":"2026100609064164700_cit22","doi-asserted-by":"publisher","first-page":"3804","DOI":"10.1038\/ncomms4804","article-title":"Chemodiversity of\ndissolved organic matter in lakes driven by climate and hydrology","volume":"5","author":"Kellerman","year":"2014","journal-title":"Nat. Commun."},{"issue":"1","key":"2026100609064164700_cit23","doi-asserted-by":"publisher","first-page":"6361","DOI":"10.1038\/s41467-025-61753-7","article-title":"Pathways and selectivity\nof fenton degradation of different precursor species of dissolved\norganic matter","volume":"16","author":"Chen","year":"2025","journal-title":"Nat. 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Sci. Technol."},{"issue":"9","key":"2026100609064164700_cit28","doi-asserted-by":"publisher","first-page":"5034","DOI":"10.1021\/acs.est.8b06333","article-title":"Humic substances facilitate arsenic\nreduction and release in flooded paddy soil","volume":"53","author":"Qiao","year":"2019","journal-title":"Environ. Sci. Technol."},{"issue":"6","key":"2026100609064164700_cit29","doi-asserted-by":"publisher","first-page":"3176","DOI":"10.1021\/acs.est.6b04131","article-title":"Increased electron-accepting and\ndecreased electron-donating capacities of soil humic substances in\nresponse to increasing temperature","volume":"51","author":"Tan","year":"2017","journal-title":"Environ.\nSci. 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Mater."},{"issue":"1","key":"2026100609064164700_cit34","doi-asserted-by":"publisher","first-page":"831","DOI":"10.1021\/acs.est.2c08482","article-title":"Unified modeling\napproach for quantifying the proton and metal binding ability of soil\ndissolved organic matter","volume":"57","author":"Ye","year":"2023","journal-title":"Environ. Sci. 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A perspective\nfrom dom molecular composition","volume":"220","author":"Huang","year":"2022","journal-title":"Water Res."},{"key":"2026100609064164700_cit39","doi-asserted-by":"publisher","first-page":"122","DOI":"10.1016\/j.gca.2025.11.041","article-title":"Dissolved organic matter oxidizes\nferrous iron and forms colloidal ternary complexes with arsenic via\nferric iron bridging in water under anoxic conditions","volume":"413","author":"Husain","year":"2026","journal-title":"Geochim. Cosmochim. Acta"},{"key":"2026100609064164700_cit40","doi-asserted-by":"publisher","first-page":"135047","DOI":"10.1016\/j.jhazmat.2024.135047","article-title":"Metagenomic\nand FT-ICR MS insights into the mechanism for the arsenic biogeochemical\ncycling in groundwater","volume":"476","author":"Jiang","year":"2024","journal-title":"J. Hazard. Mater."},{"issue":"37","key":"2026100609064164700_cit41","doi-asserted-by":"publisher","first-page":"19856","DOI":"10.1021\/acs.est.5c09633","article-title":"Microbial\nphysiological adaptation to biodegradable microplastics\ndrives the transformation and reactivity of dissolved organic matter\nin soil","volume":"59","author":"Liu","year":"2025","journal-title":"Environ. Sci. Technol."},{"key":"2026100609064164700_cit42","doi-asserted-by":"publisher","first-page":"133081","DOI":"10.1016\/j.jhazmat.2023.133081","article-title":"Natural and anthropogenic dissolved\norganic matter in landfill leachate: Composition, transformation,\nand their coexistence characteristics","volume":"465","author":"Zheng","year":"2024","journal-title":"J. Hazard.\nMater."},{"key":"2026100609064164700_cit43","doi-asserted-by":"publisher","first-page":"580","DOI":"10.1016\/j.jes.2024.12.005","article-title":"Deciphering\nthe composition and degradation\nof dissolved organic matter in a large subtropical river using optical\nindices and high-resolution FT-ICR MS","volume":"157","author":"Wang","year":"2025","journal-title":"J. Environ.\nSci."},{"issue":"1","key":"2026100609064164700_cit44","doi-asserted-by":"publisher","first-page":"187","DOI":"10.1038\/s41467-023-44431-4","article-title":"Universal\nmicrobial reworking of dissolved organic matter along environmental\ngradients","volume":"15","author":"Freeman","year":"2024","journal-title":"Nat. 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Microbiol."},{"key":"2026100609064164700_cit47","doi-asserted-by":"publisher","first-page":"100610","DOI":"10.1016\/j.ese.2025.100610","article-title":"Heavy metals\ntrigger distinct molecular transformations in microplastic-versus\nnatural-derived dissolved organic matter","volume":"27","author":"Zhong","year":"2025","journal-title":"Environ.\nSci. Ecotechnol."},{"key":"2026100609064164700_cit48","doi-asserted-by":"publisher","first-page":"159238","DOI":"10.1016\/j.cej.2025.159238","article-title":"Molecular fractionation\nduring coprecipitation of dissolved black\ncarbon with Fe(III): Preferential carbon sequestration for redox active\nmolecules","volume":"505","author":"Sun","year":"2025","journal-title":"Chem. Eng. 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