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Here, we develop a synergistic UV222\/H2O2\/Ag2O process integrating far-UVC photolysis, peroxide activation, and Ag2O catalysis within a unified Fenton-like framework. In real secondary effluent, the ternary process delivers a total organic carbon removal rate constant of 0.117 min\u20131, which is 1.8 times that of the UV222\/H2O2 system (0.065 min\u20131) and far superior than UV254-based counterparts; while enabling 7-log Escherichia coli inactivation within 6 min. The process also exhibits broad pH tolerance, resistance to anionic interference, and high operational stability. Mechanistically, H2O2 adsorbs onto Ag2O in a bidentate configuration, forming silver-coordinated hydroxyl groups (Ag2O*-*OH) that undergo hole-triggered deprotonation to yield transient interfacial high-valent AgII-oxo species. Density functional theory calculations show that hole capture lowers the deprotonation energy barrier from 2.43 to 0.67 eV, facilitating AgII-oxo formation. These nonradical oxidants operate via single-electron transfer, complementing radical pathways. The treated effluent shows improved clarity and stability, as confirmed by molecular-level analysis. Life cycle assessment and stable continuous operation with limited silver release using Ag2O-sodium alginate gel spheres demonstrate practical potential. This work highlights the critical role of photoexcited holes in advancing photo-Fenton-like catalysis for sustainable environmental remediation.<\/jats:p>","DOI":"10.1021\/acs.est.6c05171","type":"journal-article","created":{"date-parts":[[2026,9,25]],"date-time":"2026-09-25T19:02:44Z","timestamp":1790362964000},"page":"29113-29124","source":"Crossref","is-referenced-by-count":0,"title":["Silver\nOxide-Driven Far-UVC Fenton-like Wastewater\nTreatment: Hole-Induced High-Valent Silver Formation"],"prefix":"10.1021","volume":"60","author":[{"given":"Wenjun","family":"Yin","sequence":"first","affiliation":[{"name":"Hunan University , , , ,","place":["Changsha, Hunan, China, 410082"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nan","family":"Li","sequence":"additional","affiliation":[{"name":"Hunan University , , ,","place":["Changsha, China, 410082"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin","family":"Mao","sequence":"additional","affiliation":[{"name":"Hunan University , , ,","place":["Changsha, China, 410082"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juan","family":"Li","sequence":"additional","affiliation":[{"name":"Beijing Normal University , , ,","place":["Zhuhai, China, 519087"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xurui","family":"Mai","sequence":"additional","affiliation":[{"name":"The Hong Kong University of Science and Technology , , ,","place":["Hong Kong, China, 999077"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bin","family":"Liu","sequence":"additional","affiliation":[{"name":"Beijing Normal University , , ,","place":["Zhuhai, China, 519087"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4437-2060","authenticated-orcid":true,"given":"Haoran","family":"Dong","sequence":"additional","affiliation":[{"name":"Hunan University , , , ,","place":["Changsha, Hunan, China, 410082"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,25]]},"reference":[{"issue":"7","key":"2026101310154113000_cit1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202419680","article-title":"Aeration-Free\nPhoto-Fenton-Like Reaction Mediated by Heterojunction Photocatalyst\ntoward Efficient Degradation of Organic Pollutants","volume":"64","author":"Wang","year":"2025","journal-title":"Angew. Chem., Int. Ed."},{"issue":"8","key":"2026101310154113000_cit2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202318927","article-title":"Photo-self-Fenton Reaction\nMediated by Atomically Dispersed Ag-Co Photocatalysts toward Efficient\nDegradation of Organic Pollutants","volume":"63","author":"Lian","year":"2024","journal-title":"Angew. Chem.,\nInt. Ed."},{"issue":"35","key":"2026101310154113000_cit3","doi-asserted-by":"publisher","first-page":"15846","DOI":"10.1021\/acs.est.4c05181","article-title":"Control\nof Aromatic Disinfection Byproducts in Potable Reuse Water by the\nUV222\/H2O2 vs UV254\/H2O2 Advanced Oxidation Processes","volume":"58","author":"Zhao","year":"2024","journal-title":"Environ. Sci. Technol."},{"key":"2026101310154113000_cit4","doi-asserted-by":"publisher","DOI":"10.1016\/j.watres.2019.115203","article-title":"Ultrafast photodegradation of isoxazole\nand isothiazolinones by UV254 and UV254\/H2O2 photolysis in a microcapillary reactor","volume":"169","author":"Russo","year":"2020","journal-title":"Water Res."},{"key":"2026101310154113000_cit5","doi-asserted-by":"publisher","DOI":"10.1016\/j.watres.2023.120169","article-title":"Making waves: Opportunities\nand challenges\nof applying far-UVC radiation in controlling micropollutants in water","volume":"241","author":"Zhao","year":"2023","journal-title":"Water Res."},{"key":"2026101310154113000_cit6","doi-asserted-by":"publisher","DOI":"10.1016\/j.jclepro.2023.140255","article-title":"Kinetic modeling and\nmechanisms of parahalogenated phenols degradation\nby UV222\/H2O2","volume":"434","author":"Zhao","year":"2024","journal-title":"J. Clean. 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Alloys Compd."},{"issue":"8","key":"2026101310154113000_cit22","doi-asserted-by":"publisher","first-page":"684","DOI":"10.1038\/s41929-021-00659-1","article-title":"\u03b1-Fe2O3 as a versatile and efficient oxygen atom transfer\ncatalyst in combination\nwith H2O as the oxygen source","volume":"4","author":"Zhao","year":"2021","journal-title":"Nat.\nCatal."},{"issue":"n\/a","key":"2026101310154113000_cit23","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202507085","article-title":"Photoexcited Hole-Enabled Synthesis of Surface High-Valent\nCobalt-Oxo\nSpecies with Water as the Oxygen Atom Source for Water Purification","volume":"n\/a","author":"Su","year":"2025","journal-title":"Angew. Chem., Int. 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Mater."},{"key":"2026101310154113000_cit28","doi-asserted-by":"publisher","DOI":"10.1016\/j.jhazmat.2025.138099","article-title":"Efficient disinfection of real toilet\nblackwater by ultraviolet\/peracetic\nacid process: Selective intracellular biomolecular oxidation","volume":"492","author":"Yin","year":"2025","journal-title":"J. Hazard. Mater."},{"key":"2026101310154113000_cit29","doi-asserted-by":"publisher","DOI":"10.1016\/j.jphotochem.2020.113091","article-title":"Investigating\nthe influence of silver state on electronic properties of Ag\/Ag2O\/TiO2 heterojunctions prepared by photodeposition","volume":"408","author":"Vodyankin","year":"2021","journal-title":"J. Photochem. 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Horiz."},{"key":"2026101310154113000_cit32","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2024.151371","article-title":"Degradation mechanisms\nof antibiotics in UV222\/H2O2 and\nUV222\/persulfate systems: Dual roles of inorganic anions","volume":"489","author":"Zhao","year":"2024","journal-title":"Chem. Eng. J."},{"issue":"11","key":"2026101310154113000_cit33","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202421797","article-title":"Constrained Heterogeneous CoFe2O4\/ZnO\/PMS Fenton-Like\nSystem for Industrial Wastewater Remediation with Recyclability and\nZero Metal Loss","volume":"64","author":"Yang","year":"2025","journal-title":"Angew. Chem., Int. Ed."},{"issue":"22","key":"2026101310154113000_cit34","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202503901","article-title":"Leveraging Polaron Effect for Solar-Driven\nEfficient Peroxymonosulfate\nActivation in Water Purification","volume":"64","author":"Yang","year":"2025","journal-title":"Angew. Chem.,\nInt. 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