Marina Aliste , Lixy Olinda León-Morán , Carmen María Martínez-Escudero , Isabel Garrido , Fulgencio Contreras , Pilar Hellín , Pilar Flores , José Fenoll
{"title":"在中性 pH 条件下使用 Fe3+-EDDS 和 Fe3+-NTA 的太阳能光-芬顿去除废水中的布洛芬、双氯芬酸及其主要转化产物","authors":"Marina Aliste , Lixy Olinda León-Morán , Carmen María Martínez-Escudero , Isabel Garrido , Fulgencio Contreras , Pilar Hellín , Pilar Flores , José Fenoll","doi":"10.1016/j.cattod.2024.115139","DOIUrl":null,"url":null,"abstract":"<div><div>In recent years, solar photo-Fenton (SPF) processes have gained interest owing to the use of a cost-free and sustainable radiation source and their effectiveness in removing pharmaceuticals, among other Emerging Pollutants (EPs), from wastewater. Especially, when iron complexes are used to work at neutral pH. The stability and biodegradability characteristics make ethylenediamine-N,N-disuccinic acid (EDDS), and nitrilotriacetic acid (NTA) suitable iron complexing agents. In this work, the removal of diclofenac (DCF) and ibuprofen (IBU), two of the most widely used Non-steroidal Anti-Inflammatory Drug (NSAID) for the treatment of pain, at 200 µg L<sup>−1</sup> was studied in wastewater using SPF at natural pH, comparing EDDS and NTA as chelating agents for the first time. The main transformation products (TPs) were also monitored. For this purpose, a suitable analytical method using liquid chromatography coupled to triple quadrupole tandem mass spectrometry (LC-QqQ-MS/MS) with Electro Spray Ionization negative mode (ESI<sup>-</sup>) was applied to determine the pharmaceutical EPs and their main TPs in wastewater. Next, they were confirmed by LC-QTOF-HRMS. DCF was degraded 44 % faster with NTA (t<sub>1/2</sub> 53 min) than with EDDS (t<sub>1/2</sub> 77 min), although the final removal percentages, including photolysis, were similar (90–93 %). In contrast, IBU removal with EDDS (t<sub>1/2</sub> 116 min) was twice as fast as with NTA (t<sub>1/2</sub> 231 min), whereas photolysis was ineffective. Twenty TPs were monitored, of which only three were detected because of the low concentration used in this study: DCF-2C (<em>m/z</em> 258.0326), DCF-6B (<em>m/z</em> 310.0040), and IBU-4 (<em>m/z</em> 221.1181). Their behaviour followed a formation-elimination profile, but only the complete oxidation of DCF-6 was achieved. This work focuses on the kinetic aspects and TPs formed, which are useful for improving knowledge for the development of efficient processes to abate organic pollutants in real aqueous matrices. Therefore, more EPs should be thoroughly studied to determine the efficiency of EDDS and NTA as iron-chelating agents and the necessity of implementing the SPF process in WWTPs.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"446 ","pages":"Article 115139"},"PeriodicalIF":5.2000,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Solar photo-Fenton with Fe3+-EDDS and Fe3+-NTA at neutral pH for removal of ibuprofen, diclofenac and their main transformation products in wastewater\",\"authors\":\"Marina Aliste , Lixy Olinda León-Morán , Carmen María Martínez-Escudero , Isabel Garrido , Fulgencio Contreras , Pilar Hellín , Pilar Flores , José Fenoll\",\"doi\":\"10.1016/j.cattod.2024.115139\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In recent years, solar photo-Fenton (SPF) processes have gained interest owing to the use of a cost-free and sustainable radiation source and their effectiveness in removing pharmaceuticals, among other Emerging Pollutants (EPs), from wastewater. Especially, when iron complexes are used to work at neutral pH. The stability and biodegradability characteristics make ethylenediamine-N,N-disuccinic acid (EDDS), and nitrilotriacetic acid (NTA) suitable iron complexing agents. In this work, the removal of diclofenac (DCF) and ibuprofen (IBU), two of the most widely used Non-steroidal Anti-Inflammatory Drug (NSAID) for the treatment of pain, at 200 µg L<sup>−1</sup> was studied in wastewater using SPF at natural pH, comparing EDDS and NTA as chelating agents for the first time. The main transformation products (TPs) were also monitored. For this purpose, a suitable analytical method using liquid chromatography coupled to triple quadrupole tandem mass spectrometry (LC-QqQ-MS/MS) with Electro Spray Ionization negative mode (ESI<sup>-</sup>) was applied to determine the pharmaceutical EPs and their main TPs in wastewater. Next, they were confirmed by LC-QTOF-HRMS. DCF was degraded 44 % faster with NTA (t<sub>1/2</sub> 53 min) than with EDDS (t<sub>1/2</sub> 77 min), although the final removal percentages, including photolysis, were similar (90–93 %). In contrast, IBU removal with EDDS (t<sub>1/2</sub> 116 min) was twice as fast as with NTA (t<sub>1/2</sub> 231 min), whereas photolysis was ineffective. Twenty TPs were monitored, of which only three were detected because of the low concentration used in this study: DCF-2C (<em>m/z</em> 258.0326), DCF-6B (<em>m/z</em> 310.0040), and IBU-4 (<em>m/z</em> 221.1181). Their behaviour followed a formation-elimination profile, but only the complete oxidation of DCF-6 was achieved. This work focuses on the kinetic aspects and TPs formed, which are useful for improving knowledge for the development of efficient processes to abate organic pollutants in real aqueous matrices. Therefore, more EPs should be thoroughly studied to determine the efficiency of EDDS and NTA as iron-chelating agents and the necessity of implementing the SPF process in WWTPs.</div></div>\",\"PeriodicalId\":264,\"journal\":{\"name\":\"Catalysis Today\",\"volume\":\"446 \",\"pages\":\"Article 115139\"},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2024-11-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Today\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0920586124006333\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Today","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0920586124006333","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Solar photo-Fenton with Fe3+-EDDS and Fe3+-NTA at neutral pH for removal of ibuprofen, diclofenac and their main transformation products in wastewater
In recent years, solar photo-Fenton (SPF) processes have gained interest owing to the use of a cost-free and sustainable radiation source and their effectiveness in removing pharmaceuticals, among other Emerging Pollutants (EPs), from wastewater. Especially, when iron complexes are used to work at neutral pH. The stability and biodegradability characteristics make ethylenediamine-N,N-disuccinic acid (EDDS), and nitrilotriacetic acid (NTA) suitable iron complexing agents. In this work, the removal of diclofenac (DCF) and ibuprofen (IBU), two of the most widely used Non-steroidal Anti-Inflammatory Drug (NSAID) for the treatment of pain, at 200 µg L−1 was studied in wastewater using SPF at natural pH, comparing EDDS and NTA as chelating agents for the first time. The main transformation products (TPs) were also monitored. For this purpose, a suitable analytical method using liquid chromatography coupled to triple quadrupole tandem mass spectrometry (LC-QqQ-MS/MS) with Electro Spray Ionization negative mode (ESI-) was applied to determine the pharmaceutical EPs and their main TPs in wastewater. Next, they were confirmed by LC-QTOF-HRMS. DCF was degraded 44 % faster with NTA (t1/2 53 min) than with EDDS (t1/2 77 min), although the final removal percentages, including photolysis, were similar (90–93 %). In contrast, IBU removal with EDDS (t1/2 116 min) was twice as fast as with NTA (t1/2 231 min), whereas photolysis was ineffective. Twenty TPs were monitored, of which only three were detected because of the low concentration used in this study: DCF-2C (m/z 258.0326), DCF-6B (m/z 310.0040), and IBU-4 (m/z 221.1181). Their behaviour followed a formation-elimination profile, but only the complete oxidation of DCF-6 was achieved. This work focuses on the kinetic aspects and TPs formed, which are useful for improving knowledge for the development of efficient processes to abate organic pollutants in real aqueous matrices. Therefore, more EPs should be thoroughly studied to determine the efficiency of EDDS and NTA as iron-chelating agents and the necessity of implementing the SPF process in WWTPs.
期刊介绍:
Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues.
Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.