Yuexinxi Wang , Yong Liu , Shizong Wang , Jingwen Wang , Jianlong Wang
{"title":"新型催化臭氧氧化系统对氨氮的选择性氧化:亚硫酸盐对氮气选择性的调节。","authors":"Yuexinxi Wang , Yong Liu , Shizong Wang , Jingwen Wang , Jianlong Wang","doi":"10.1016/j.chemosphere.2024.143999","DOIUrl":null,"url":null,"abstract":"<div><div>The selective oxidation of NH<sub>4</sub><sup>+</sup>-N into dinitrogen (N<sub>2</sub>) is still a challenge. Currently, traditional advanced oxidation processes often involve in the chlorine free radicals to increase the selectivity of NH<sub>4</sub><sup>+</sup>-N oxidation products towards N<sub>2</sub> but is usually accompanied by the production of many toxic disinfection by-product. Herein, we reported a novel catalytic ozonation system (UV/O<sub>3</sub>/MgO/Na<sub>2</sub>SO<sub>3</sub>) for selective NH<sub>4</sub><sup>+</sup>-N oxidation based on the reducing capability and photochemical properties of Na<sub>2</sub>SO<sub>3</sub>. In the UV/O<sub>3</sub>/MgO/Na<sub>2</sub>SO<sub>3</sub>/NH<sub>4</sub><sup>+</sup>-N system, Na<sub>2</sub>SO<sub>3</sub> could not only reduce the intermediate of NO<sub>2</sub><sup>−</sup> or NO<sub>3</sub><sup>−</sup> to N<sub>2</sub> by inducing the generation of hydrated electrons under UV irradiation, but also reduce the gaseous intermediate of NO<sub>x</sub> to N<sub>2</sub>, thus achieving a high N<sub>2</sub> selectivity (>85 %). Based on the analyses of each component roles, the determination of reactive oxygen species and the evolution of NH<sub>4</sub><sup>+</sup>-N oxidation intermediates, the possible mechanisms of NH<sub>4</sub><sup>+</sup>-N selective oxidation by UV/O<sub>3</sub>/MgO/Na<sub>2</sub>SO<sub>3</sub> system were revealed. This system exhibits a great potential for the NH<sub>4</sub><sup>+</sup>-N removal from water/wastewater. This work provides a new strategy for NH<sub>4</sub><sup>+</sup>-N oxidation into N<sub>2</sub> by advanced oxidation processes independent of the action of chlorine free radicals.</div></div>","PeriodicalId":276,"journal":{"name":"Chemosphere","volume":"370 ","pages":"Article 143999"},"PeriodicalIF":8.1000,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective oxidation of ammonium to dinitrogen by a novel catalytic ozonation system: Regulating the N2 selectivity by sulfite\",\"authors\":\"Yuexinxi Wang , Yong Liu , Shizong Wang , Jingwen Wang , Jianlong Wang\",\"doi\":\"10.1016/j.chemosphere.2024.143999\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The selective oxidation of NH<sub>4</sub><sup>+</sup>-N into dinitrogen (N<sub>2</sub>) is still a challenge. Currently, traditional advanced oxidation processes often involve in the chlorine free radicals to increase the selectivity of NH<sub>4</sub><sup>+</sup>-N oxidation products towards N<sub>2</sub> but is usually accompanied by the production of many toxic disinfection by-product. Herein, we reported a novel catalytic ozonation system (UV/O<sub>3</sub>/MgO/Na<sub>2</sub>SO<sub>3</sub>) for selective NH<sub>4</sub><sup>+</sup>-N oxidation based on the reducing capability and photochemical properties of Na<sub>2</sub>SO<sub>3</sub>. In the UV/O<sub>3</sub>/MgO/Na<sub>2</sub>SO<sub>3</sub>/NH<sub>4</sub><sup>+</sup>-N system, Na<sub>2</sub>SO<sub>3</sub> could not only reduce the intermediate of NO<sub>2</sub><sup>−</sup> or NO<sub>3</sub><sup>−</sup> to N<sub>2</sub> by inducing the generation of hydrated electrons under UV irradiation, but also reduce the gaseous intermediate of NO<sub>x</sub> to N<sub>2</sub>, thus achieving a high N<sub>2</sub> selectivity (>85 %). Based on the analyses of each component roles, the determination of reactive oxygen species and the evolution of NH<sub>4</sub><sup>+</sup>-N oxidation intermediates, the possible mechanisms of NH<sub>4</sub><sup>+</sup>-N selective oxidation by UV/O<sub>3</sub>/MgO/Na<sub>2</sub>SO<sub>3</sub> system were revealed. This system exhibits a great potential for the NH<sub>4</sub><sup>+</sup>-N removal from water/wastewater. This work provides a new strategy for NH<sub>4</sub><sup>+</sup>-N oxidation into N<sub>2</sub> by advanced oxidation processes independent of the action of chlorine free radicals.</div></div>\",\"PeriodicalId\":276,\"journal\":{\"name\":\"Chemosphere\",\"volume\":\"370 \",\"pages\":\"Article 143999\"},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2025-02-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemosphere\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0045653524029072\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemosphere","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0045653524029072","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
Selective oxidation of ammonium to dinitrogen by a novel catalytic ozonation system: Regulating the N2 selectivity by sulfite
The selective oxidation of NH4+-N into dinitrogen (N2) is still a challenge. Currently, traditional advanced oxidation processes often involve in the chlorine free radicals to increase the selectivity of NH4+-N oxidation products towards N2 but is usually accompanied by the production of many toxic disinfection by-product. Herein, we reported a novel catalytic ozonation system (UV/O3/MgO/Na2SO3) for selective NH4+-N oxidation based on the reducing capability and photochemical properties of Na2SO3. In the UV/O3/MgO/Na2SO3/NH4+-N system, Na2SO3 could not only reduce the intermediate of NO2− or NO3− to N2 by inducing the generation of hydrated electrons under UV irradiation, but also reduce the gaseous intermediate of NOx to N2, thus achieving a high N2 selectivity (>85 %). Based on the analyses of each component roles, the determination of reactive oxygen species and the evolution of NH4+-N oxidation intermediates, the possible mechanisms of NH4+-N selective oxidation by UV/O3/MgO/Na2SO3 system were revealed. This system exhibits a great potential for the NH4+-N removal from water/wastewater. This work provides a new strategy for NH4+-N oxidation into N2 by advanced oxidation processes independent of the action of chlorine free radicals.
期刊介绍:
Chemosphere, being an international multidisciplinary journal, is dedicated to publishing original communications and review articles on chemicals in the environment. The scope covers a wide range of topics, including the identification, quantification, behavior, fate, toxicology, treatment, and remediation of chemicals in the bio-, hydro-, litho-, and atmosphere, ensuring the broad dissemination of research in this field.