Jiaqi Ren , Ying Huang , Jiani Yao , Shujie Zheng , Yingjie Zhao , Yang Hou , Bin Yang , Lecheng Lei , Zhongjian Li , Dionysios D. Dionysiou
{"title":"活性磷酸盐在活化过氧单硫酸盐处理富磷废水中减少微污染物中的作用","authors":"Jiaqi Ren , Ying Huang , Jiani Yao , Shujie Zheng , Yingjie Zhao , Yang Hou , Bin Yang , Lecheng Lei , Zhongjian Li , Dionysios D. Dionysiou","doi":"10.1016/j.watres.2023.120341","DOIUrl":null,"url":null,"abstract":"<div><p><span>This study investigated the mechanisms of forming reactive species to degrade micropollutants through the activation of peroxymonosulfate (PMS) by phosphate, a prevalent ion in wastewater. Considering the density functional theory results, the formation of hydrogen bonds between phosphate and PMS molecules might be the crucial step in the overall reactions, which prefers producing </span><sup>⋅</sup>OH and reactive phosphate species (RPS, namely H<sub>2</sub>PO<sub>4</sub><sup>⋅</sup>, HPO<sub>4</sub><sup>⋅−</sup>, and PO<sub>4</sub><sup>⋅2−</sup>) to yielding SO<sub>4</sub><sup>⋅−</sup>. Besides, in the phosphate (5 mM)/PMS system at pH = 8, HPO<sub>4</sub><sup>⋅−</sup> was modeled to be the dominant radical with a steady-state concentration of 3.6 × 10<sup>−12</sup> M, which was 666 and 773 times higher than those of <sup>⋅</sup>OH and SO<sub>4</sub><sup>⋅−</sup>. The contributions of <sup>1</sup>O<sub>2</sub>, <sup>⋅</sup>OH, SO<sub>4</sub><sup>⋅−</sup>, and RPS to the micropollutant decomposition in phosphate/PMS were studied, and RPS were found to be selective for micropollutants with electron-donating moieties (such as phenolic and aniline groups). Additionally, the degradation pathways of bisphenol A, diclofenac, ibuprofen, and atrazine in phosphate/PMS were proposed according to the detected transformation products. Cytotoxicity analysis was carried out to evaluate the potential environmental impacts resulting from the degradation of micropollutants by phosphate/PMS. This study confirmed the significance of RPS for micropollutant degradation during PMS-based treatment in phosphate-rich scenarios.</p></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":11.4000,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"4","resultStr":"{\"title\":\"The role of reactive phosphate species in the abatement of micropollutants by activated peroxymonosulfate in the treatment of phosphate-rich wastewater\",\"authors\":\"Jiaqi Ren , Ying Huang , Jiani Yao , Shujie Zheng , Yingjie Zhao , Yang Hou , Bin Yang , Lecheng Lei , Zhongjian Li , Dionysios D. Dionysiou\",\"doi\":\"10.1016/j.watres.2023.120341\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p><span>This study investigated the mechanisms of forming reactive species to degrade micropollutants through the activation of peroxymonosulfate (PMS) by phosphate, a prevalent ion in wastewater. Considering the density functional theory results, the formation of hydrogen bonds between phosphate and PMS molecules might be the crucial step in the overall reactions, which prefers producing </span><sup>⋅</sup>OH and reactive phosphate species (RPS, namely H<sub>2</sub>PO<sub>4</sub><sup>⋅</sup>, HPO<sub>4</sub><sup>⋅−</sup>, and PO<sub>4</sub><sup>⋅2−</sup>) to yielding SO<sub>4</sub><sup>⋅−</sup>. Besides, in the phosphate (5 mM)/PMS system at pH = 8, HPO<sub>4</sub><sup>⋅−</sup> was modeled to be the dominant radical with a steady-state concentration of 3.6 × 10<sup>−12</sup> M, which was 666 and 773 times higher than those of <sup>⋅</sup>OH and SO<sub>4</sub><sup>⋅−</sup>. The contributions of <sup>1</sup>O<sub>2</sub>, <sup>⋅</sup>OH, SO<sub>4</sub><sup>⋅−</sup>, and RPS to the micropollutant decomposition in phosphate/PMS were studied, and RPS were found to be selective for micropollutants with electron-donating moieties (such as phenolic and aniline groups). Additionally, the degradation pathways of bisphenol A, diclofenac, ibuprofen, and atrazine in phosphate/PMS were proposed according to the detected transformation products. Cytotoxicity analysis was carried out to evaluate the potential environmental impacts resulting from the degradation of micropollutants by phosphate/PMS. This study confirmed the significance of RPS for micropollutant degradation during PMS-based treatment in phosphate-rich scenarios.</p></div>\",\"PeriodicalId\":443,\"journal\":{\"name\":\"Water Research\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":11.4000,\"publicationDate\":\"2023-09-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"4\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Water Research\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0043135423007777\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Water Research","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0043135423007777","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
The role of reactive phosphate species in the abatement of micropollutants by activated peroxymonosulfate in the treatment of phosphate-rich wastewater
This study investigated the mechanisms of forming reactive species to degrade micropollutants through the activation of peroxymonosulfate (PMS) by phosphate, a prevalent ion in wastewater. Considering the density functional theory results, the formation of hydrogen bonds between phosphate and PMS molecules might be the crucial step in the overall reactions, which prefers producing ⋅OH and reactive phosphate species (RPS, namely H2PO4⋅, HPO4⋅−, and PO4⋅2−) to yielding SO4⋅−. Besides, in the phosphate (5 mM)/PMS system at pH = 8, HPO4⋅− was modeled to be the dominant radical with a steady-state concentration of 3.6 × 10−12 M, which was 666 and 773 times higher than those of ⋅OH and SO4⋅−. The contributions of 1O2, ⋅OH, SO4⋅−, and RPS to the micropollutant decomposition in phosphate/PMS were studied, and RPS were found to be selective for micropollutants with electron-donating moieties (such as phenolic and aniline groups). Additionally, the degradation pathways of bisphenol A, diclofenac, ibuprofen, and atrazine in phosphate/PMS were proposed according to the detected transformation products. Cytotoxicity analysis was carried out to evaluate the potential environmental impacts resulting from the degradation of micropollutants by phosphate/PMS. This study confirmed the significance of RPS for micropollutant degradation during PMS-based treatment in phosphate-rich scenarios.
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.