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氨基羧酸盐螯合钴活化过一硫酸盐降解四环素

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以氨基羧酸盐为螯合剂制备了一种良好的金属基非均相催化剂。在室温和酸性pH条件下(pH~6),将氨基羧酸盐亚氨基二琥珀酸四钠(IDS)螯合金属钴并接枝在壳聚糖(CS)上制备了复合催化剂(CSI-Co)。通过EDS能谱仪,傅立叶红外光谱仪(FT-IR),X射线光电子能谱仪(XPS)等表征结果表明,CS和IDS成功接枝形成酰胺键,同时金属Co也成功螯合到复合材料上。利用CSI-Co活化过一硫酸盐(PMS)降解盐酸四环素(TCH),在10mg/L TCH(初始pH~5。21),PMS投加量为400mg/L,CSI-Co投加量为200mg/L的条件下,反应10min TCH的降解率达98。52%,且重复使用4次后降解率仍达74。16%。在较宽pH范围内(3~11),多种阴离子(HCO3-,HPO42-,SO42-,Cr,NO3-)和腐殖酸(HA)存在下也有较好的催化效果,表明其优良的催化性能。通过自由基淬灭和电子顺磁共振(EPR)实验对反应体系中的活性物种进行鉴定,证实PMS/CSI-Co体系降解TCH过程中主要活性物种为单线态氧(1O2),同时少量硫酸根自由基(SO4'-)和羟基自由基(HO·)参与降解。研究结果为金属基非均相催化剂降解废水中的抗生素提供了一种新思路,表明所制备的CSI-Co在过硫酸盐催化反应及抗生素的去除中具有潜力。
Aminocarboxylate chelated cobalt activates peroxymonosulfate to degrade tetracycline
In this study,a high-quality metal-based heterogeneous catalyst was synthesized using aminocarboxylate as a chelating agent.A composite catalyst(CSI-Co)was fabricated by chelating the metal cobalt with aminocarboxylate tetrasodium iminodisuccinate(IDS)and grafting it onto chitosan(CS)at room temperature and under acidic conditions(pH~6).The results of EDS,FT-IR and X-ray photoelectron spectroscopy(XPS)showed that CS and IDS were successfully grafted to form amide bonds and Co was also successfully chelated to the composite material.Tetracycline hydrochloride(TCH)was degraded by peroxymonosulfate(PMS)activated by CSI-Co.Under the conditions of 10mg/L TCH(initial pH~5.21),PMS dosage of 400mg/L,and CSI-Co dosage of 200mg/L,the degradation rate of TCH was 98.52%after 10min reaction,and the degradation rate was still 74.16%after repeated use for 4times.It also has good catalytic effect in a wide pH range(3~11)and in the presence of multiple anions(HCO3-,HPO42-,SO42-,Cl-and NO3-)and humic acid(HA),indicating its excellent catalytic performance.The active species in the reaction system were identified by free radical quenching and electron paramagnetic resonance(EPR)experiments.It was confirmed that the main active species in the degradation of TCH by PMS/CSI-Co system was singlet oxygen(1O2),and a small amount of sulfate radical(SO4·-)and hydroxyl radical(HO')were involved in the degradation.The results provide a new idea for the preparation of metal-based heterogeneous catalysts,indicating that the prepared CSI-Co has potential in persulfate catalytic reaction and antibiotic removal.

chitosantetrasodium iminodisuccinatechelationperoxymonosulfatetetracycline

郑晓晓、李兴发、张峰、潘寒风、林嘉伟

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太原理工大学环境科学与工程学院,山西晋中 030600

壳聚糖 亚氨基二琥珀酸四钠 螯合 过一硫酸盐 四环素

山西省自然科学基金

20210302123174

2024

中国环境科学
中国环境科学学会

中国环境科学

CSTPCDCHSSCD北大核心
影响因子:2.174
ISSN:1000-6923
年,卷(期):2024.44(5)