Xue Zhang, Kang Zhang, Ting Li, Yujiao Wang and Yin Xu
{"title":"CuFe-LDHs 激活的过硫酸盐在水中降解氧氟沙星的性能和机理","authors":"Xue Zhang, Kang Zhang, Ting Li, Yujiao Wang and Yin Xu","doi":"10.1039/D4EN00370E","DOIUrl":null,"url":null,"abstract":"<p >Antibiotic-containing refractory organic wastewater is difficult to degrade <em>via</em> traditional physicochemical treatment technology because of its high stability. Therefore, an advanced oxidation process based on sulfate radicals was developed and received extensive attention because of its wider pH operating range and stronger oxidizing property, considering that the PS was easily activated by transition metals without excessive energy input. In this study, a layered double hydroxide (LDH) catalyst consisting of Cu(<small>II</small>) and Fe(<small>III</small>) (CuFe-LDHs) was synthesized to activate PS to degrade ofloxacin (OFL) in water effectively. The results showed that when the dosages of CuFe-LDHs and PS were set as 0.5 g L<small><sup>−1</sup></small> and 0.2 mM, respectively, the degradation efficiency of OFL was up to ∼80% within a wide pH operating range (3–11) and with low activation energy (<em>E</em><small><sub>a</sub></small> = 54.95 kJ mol<small><sup>−1</sup></small>) under the condition that the initial OFL concentration was 10 mg L<small><sup>−1</sup></small>. Interference experiments on OFL degradation demonstrated that Cl<small><sup>−</sup></small>, NO<small><sub>3</sub></small><small><sup>−</sup></small>, humic acid and HCO<small><sub>3</sub></small><small><sup>−</sup></small> have almost no influence on the CuFe-LDHs/PS system, while the OFL degradation performance was significantly inhibited with increasing concentration of SO<small><sub>4</sub></small><small><sup>2−</sup></small> and H<small><sub>2</sub></small>PO<small><sub>4</sub></small><small><sup>−</sup></small> (the degradation efficiency decreased by 44.4% and 60.1%, respectively). The results of quenching experiments and electron paramagnetic resonance analysis showed that SO<small><sub>4</sub></small>·<small><sup>−</sup></small> was the dominant free radical for OFL degradation, and SO<small><sub>4</sub></small>·<small><sup>−</sup></small> was generated <em>via</em> Cu-Fe electron transfer with surface-OH acting as active sites. That was the reason why the catalytic reaction process was easily affected by SO<small><sub>4</sub></small><small><sup>2−</sup></small> and H<small><sub>2</sub></small>PO<small><sub>4</sub></small><small><sup>−</sup></small>. In addition, the CuFe-LDHs/PS system exhibited excellent cycle performance: the OFL degradation efficiency remained at 66.8% after five cycles. In summary, this study provides theoretical and technical guidance for the application of CuFe-LDHs in antibiotic wastewater degradation by activating PS.</p>","PeriodicalId":73,"journal":{"name":"Environmental Science: Nano","volume":null,"pages":null},"PeriodicalIF":5.8000,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The performance and mechanism of persulfate activated by CuFe-LDHs for ofloxacin degradation in water†\",\"authors\":\"Xue Zhang, Kang Zhang, Ting Li, Yujiao Wang and Yin Xu\",\"doi\":\"10.1039/D4EN00370E\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Antibiotic-containing refractory organic wastewater is difficult to degrade <em>via</em> traditional physicochemical treatment technology because of its high stability. Therefore, an advanced oxidation process based on sulfate radicals was developed and received extensive attention because of its wider pH operating range and stronger oxidizing property, considering that the PS was easily activated by transition metals without excessive energy input. In this study, a layered double hydroxide (LDH) catalyst consisting of Cu(<small>II</small>) and Fe(<small>III</small>) (CuFe-LDHs) was synthesized to activate PS to degrade ofloxacin (OFL) in water effectively. The results showed that when the dosages of CuFe-LDHs and PS were set as 0.5 g L<small><sup>−1</sup></small> and 0.2 mM, respectively, the degradation efficiency of OFL was up to ∼80% within a wide pH operating range (3–11) and with low activation energy (<em>E</em><small><sub>a</sub></small> = 54.95 kJ mol<small><sup>−1</sup></small>) under the condition that the initial OFL concentration was 10 mg L<small><sup>−1</sup></small>. Interference experiments on OFL degradation demonstrated that Cl<small><sup>−</sup></small>, NO<small><sub>3</sub></small><small><sup>−</sup></small>, humic acid and HCO<small><sub>3</sub></small><small><sup>−</sup></small> have almost no influence on the CuFe-LDHs/PS system, while the OFL degradation performance was significantly inhibited with increasing concentration of SO<small><sub>4</sub></small><small><sup>2−</sup></small> and H<small><sub>2</sub></small>PO<small><sub>4</sub></small><small><sup>−</sup></small> (the degradation efficiency decreased by 44.4% and 60.1%, respectively). The results of quenching experiments and electron paramagnetic resonance analysis showed that SO<small><sub>4</sub></small>·<small><sup>−</sup></small> was the dominant free radical for OFL degradation, and SO<small><sub>4</sub></small>·<small><sup>−</sup></small> was generated <em>via</em> Cu-Fe electron transfer with surface-OH acting as active sites. That was the reason why the catalytic reaction process was easily affected by SO<small><sub>4</sub></small><small><sup>2−</sup></small> and H<small><sub>2</sub></small>PO<small><sub>4</sub></small><small><sup>−</sup></small>. In addition, the CuFe-LDHs/PS system exhibited excellent cycle performance: the OFL degradation efficiency remained at 66.8% after five cycles. In summary, this study provides theoretical and technical guidance for the application of CuFe-LDHs in antibiotic wastewater degradation by activating PS.</p>\",\"PeriodicalId\":73,\"journal\":{\"name\":\"Environmental Science: Nano\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-07-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Science: Nano\",\"FirstCategoryId\":\"6\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/en/d4en00370e\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Science: Nano","FirstCategoryId":"6","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/en/d4en00370e","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
The performance and mechanism of persulfate activated by CuFe-LDHs for ofloxacin degradation in water†
Antibiotic-containing refractory organic wastewater is difficult to degrade via traditional physicochemical treatment technology because of its high stability. Therefore, an advanced oxidation process based on sulfate radicals was developed and received extensive attention because of its wider pH operating range and stronger oxidizing property, considering that the PS was easily activated by transition metals without excessive energy input. In this study, a layered double hydroxide (LDH) catalyst consisting of Cu(II) and Fe(III) (CuFe-LDHs) was synthesized to activate PS to degrade ofloxacin (OFL) in water effectively. The results showed that when the dosages of CuFe-LDHs and PS were set as 0.5 g L−1 and 0.2 mM, respectively, the degradation efficiency of OFL was up to ∼80% within a wide pH operating range (3–11) and with low activation energy (Ea = 54.95 kJ mol−1) under the condition that the initial OFL concentration was 10 mg L−1. Interference experiments on OFL degradation demonstrated that Cl−, NO3−, humic acid and HCO3− have almost no influence on the CuFe-LDHs/PS system, while the OFL degradation performance was significantly inhibited with increasing concentration of SO42− and H2PO4− (the degradation efficiency decreased by 44.4% and 60.1%, respectively). The results of quenching experiments and electron paramagnetic resonance analysis showed that SO4·− was the dominant free radical for OFL degradation, and SO4·− was generated via Cu-Fe electron transfer with surface-OH acting as active sites. That was the reason why the catalytic reaction process was easily affected by SO42− and H2PO4−. In addition, the CuFe-LDHs/PS system exhibited excellent cycle performance: the OFL degradation efficiency remained at 66.8% after five cycles. In summary, this study provides theoretical and technical guidance for the application of CuFe-LDHs in antibiotic wastewater degradation by activating PS.
期刊介绍:
Environmental Science: Nano serves as a comprehensive and high-impact peer-reviewed source of information on the design and demonstration of engineered nanomaterials for environment-based applications. It also covers the interactions between engineered, natural, and incidental nanomaterials with biological and environmental systems. This scope includes, but is not limited to, the following topic areas:
Novel nanomaterial-based applications for water, air, soil, food, and energy sustainability
Nanomaterial interactions with biological systems and nanotoxicology
Environmental fate, reactivity, and transformations of nanoscale materials
Nanoscale processes in the environment
Sustainable nanotechnology including rational nanomaterial design, life cycle assessment, risk/benefit analysis