Selective elimination of organic pollutants and analysis of effects and novel mechanisms of aged microplastics on wavelength-dependent UV-LED/H2O2 system
{"title":"Selective elimination of organic pollutants and analysis of effects and novel mechanisms of aged microplastics on wavelength-dependent UV-LED/H2O2 system","authors":"","doi":"10.1016/j.watres.2024.122526","DOIUrl":null,"url":null,"abstract":"<div><div>The selective removal of organic pollutants and potential impact of aged microplastics (MPs) as emerging pollutants in wavelength-dependent UV-LED/H<sub>2</sub>O<sub>2</sub> system are not fully understood. This study found that cefalexin (CFX) degradation efficiency in UV-LED alone system was highly correlated with its UV molar absorbance (<em>R<sup>2</sup></em>=0.994), while in UV-LED/H<sub>2</sub>O<sub>2</sub> system, it was correlated with ·OH yield (<em>R<sup>2</sup></em>=0.991) across various wavelengths. Quantitative structure-activity relationship (QSAR) analysis showed selective degradation of six pollutants based on their e<sup>-</sup>-donating capabilities (<em>R<sup>2</sup></em>=0.748–0.916). The coexistence of aged MPs, introducing C-O/C=O groups and rearranging their surface e<sup>-</sup>, potentially affected the elimination efficiency of CFX. Aged polystyrene (PS) decreased the degradation efficiency of CFX by shorting the O-O bond length (<em>l<sub>O-O</sub></em>) in H<sub>2</sub>O<sub>2</sub> and capturing e<sup>-</sup> from H<sub>2</sub>O<sub>2</sub>, whereas aged polyethylene (PE), polypropylene (PP) and polyvinyl chloride (PVC) had negligible effects as the <em>l<sub>O-O</sub></em> elongation balanced the e<sup>-</sup>-donating effect of H<sub>2</sub>O<sub>2</sub>. Additionally, phenol released from aged PS, with strong nucleophilicity, competing with CFX for ·OH, further decreasing CFX degradation efficiency. This study provides valuable insights into organic pollutant selective removal and reveals a novel inhibitory mechanism of aged PS on the performance of UV-LED/H<sub>2</sub>O<sub>2</sub> technology.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":11.4000,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Water Research","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0043135424014258","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}
引用次数: 0
Abstract
The selective removal of organic pollutants and potential impact of aged microplastics (MPs) as emerging pollutants in wavelength-dependent UV-LED/H2O2 system are not fully understood. This study found that cefalexin (CFX) degradation efficiency in UV-LED alone system was highly correlated with its UV molar absorbance (R2=0.994), while in UV-LED/H2O2 system, it was correlated with ·OH yield (R2=0.991) across various wavelengths. Quantitative structure-activity relationship (QSAR) analysis showed selective degradation of six pollutants based on their e--donating capabilities (R2=0.748–0.916). The coexistence of aged MPs, introducing C-O/C=O groups and rearranging their surface e-, potentially affected the elimination efficiency of CFX. Aged polystyrene (PS) decreased the degradation efficiency of CFX by shorting the O-O bond length (lO-O) in H2O2 and capturing e- from H2O2, whereas aged polyethylene (PE), polypropylene (PP) and polyvinyl chloride (PVC) had negligible effects as the lO-O elongation balanced the e--donating effect of H2O2. Additionally, phenol released from aged PS, with strong nucleophilicity, competing with CFX for ·OH, further decreasing CFX degradation efficiency. This study provides valuable insights into organic pollutant selective removal and reveals a novel inhibitory mechanism of aged PS on the performance of UV-LED/H2O2 technology.
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.
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