Wenxin Shi, Chi Zhang, He Zhao, Heli Tang, Yanan Liu, Bing Zhang
{"title":"低紫外剂量,高效率:远紫外vc和高铁酸盐(VI)的协同耦合超快选择性降解微污染物","authors":"Wenxin Shi, Chi Zhang, He Zhao, Heli Tang, Yanan Liu, Bing Zhang","doi":"10.1016/j.watres.2025.123785","DOIUrl":null,"url":null,"abstract":"Enhancing the reactivity and yield of reactive species to reduce the ultraviolet (UV) fluence requirement for activating ferrate (Fe(VI)) is critical for advancing UV-based Fe(VI) processes toward practical wastewater treatment applications, yet it remains challenging. Herein, we developed a far-UVC-driven Fe(VI) activation system for the efficient degradation of micropollutants. The results demonstrated that switching from conventional low-pressure UV lamps (LPUV, UV<sub>254</sub>) and UVA<sub>365</sub> to 222 nm far-UVC achieved ultrafast degradation of carbamazepine (CBZ) at an extremely low UV dose of 29.76 mJ/cm<sup>2</sup> under pH 8.0 conditions. The fluence-based degradation rate constants were 15.8 and 142.0 times higher than those achieved by UV<sub>254</sub> and UVA<sub>365</sub> photolysis of Fe(VI), respectively. This improved degradation can be attributed to the increased generation of high-valent iron intermediates [(Fe(V)/Fe(IV)] in the system. Notably, the presence of complex matrixes barely influenced CBZ degradation, and the UV<sub>222</sub>/Fe(VI) system maintained significantly enhanced performance in various real waters compared to Fe(VI) alone. Additionally, 10 structurally diverse pollutants were selected for evaluation the selectivity of the UV<sub>222</sub>/Fe(VI) system, finding that their ln<em>k<sub>obs</sub></em> values correlated well with their E<sub>HOMO</sub> and vertical IP (<em>R</em><sup>2</sup> = 0.86). Overall, this study proposes a promising oxidation technology that was efficient, energy-saving, cost-effective, and selective for the rapid elimination of micropollutants.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"1 1","pages":""},"PeriodicalIF":11.4000,"publicationDate":"2025-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Low ultraviolet dose with high efficiency: Synergistic coupling of far-UVC and ferrate(VI) for ultrafast and selective degradation of micropollutants\",\"authors\":\"Wenxin Shi, Chi Zhang, He Zhao, Heli Tang, Yanan Liu, Bing Zhang\",\"doi\":\"10.1016/j.watres.2025.123785\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Enhancing the reactivity and yield of reactive species to reduce the ultraviolet (UV) fluence requirement for activating ferrate (Fe(VI)) is critical for advancing UV-based Fe(VI) processes toward practical wastewater treatment applications, yet it remains challenging. Herein, we developed a far-UVC-driven Fe(VI) activation system for the efficient degradation of micropollutants. The results demonstrated that switching from conventional low-pressure UV lamps (LPUV, UV<sub>254</sub>) and UVA<sub>365</sub> to 222 nm far-UVC achieved ultrafast degradation of carbamazepine (CBZ) at an extremely low UV dose of 29.76 mJ/cm<sup>2</sup> under pH 8.0 conditions. The fluence-based degradation rate constants were 15.8 and 142.0 times higher than those achieved by UV<sub>254</sub> and UVA<sub>365</sub> photolysis of Fe(VI), respectively. This improved degradation can be attributed to the increased generation of high-valent iron intermediates [(Fe(V)/Fe(IV)] in the system. Notably, the presence of complex matrixes barely influenced CBZ degradation, and the UV<sub>222</sub>/Fe(VI) system maintained significantly enhanced performance in various real waters compared to Fe(VI) alone. Additionally, 10 structurally diverse pollutants were selected for evaluation the selectivity of the UV<sub>222</sub>/Fe(VI) system, finding that their ln<em>k<sub>obs</sub></em> values correlated well with their E<sub>HOMO</sub> and vertical IP (<em>R</em><sup>2</sup> = 0.86). 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Low ultraviolet dose with high efficiency: Synergistic coupling of far-UVC and ferrate(VI) for ultrafast and selective degradation of micropollutants
Enhancing the reactivity and yield of reactive species to reduce the ultraviolet (UV) fluence requirement for activating ferrate (Fe(VI)) is critical for advancing UV-based Fe(VI) processes toward practical wastewater treatment applications, yet it remains challenging. Herein, we developed a far-UVC-driven Fe(VI) activation system for the efficient degradation of micropollutants. The results demonstrated that switching from conventional low-pressure UV lamps (LPUV, UV254) and UVA365 to 222 nm far-UVC achieved ultrafast degradation of carbamazepine (CBZ) at an extremely low UV dose of 29.76 mJ/cm2 under pH 8.0 conditions. The fluence-based degradation rate constants were 15.8 and 142.0 times higher than those achieved by UV254 and UVA365 photolysis of Fe(VI), respectively. This improved degradation can be attributed to the increased generation of high-valent iron intermediates [(Fe(V)/Fe(IV)] in the system. Notably, the presence of complex matrixes barely influenced CBZ degradation, and the UV222/Fe(VI) system maintained significantly enhanced performance in various real waters compared to Fe(VI) alone. Additionally, 10 structurally diverse pollutants were selected for evaluation the selectivity of the UV222/Fe(VI) system, finding that their lnkobs values correlated well with their EHOMO and vertical IP (R2 = 0.86). Overall, this study proposes a promising oxidation technology that was efficient, energy-saving, cost-effective, and selective for the rapid elimination of micropollutants.
期刊介绍:
Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include:
•Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management;
•Urban hydrology including sewer systems, stormwater management, and green infrastructure;
•Drinking water treatment and distribution;
•Potable and non-potable water reuse;
•Sanitation, public health, and risk assessment;
•Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions;
•Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment;
•Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution;
•Environmental restoration, linked to surface water, groundwater and groundwater remediation;
•Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts;
•Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle;
•Socio-economic, policy, and regulations studies.