• 关键词：卡巴多司  奥喹多司  过硫酸盐  硫酸根自由基  降解

• 基金项目：国家自然科学基金（No.21607077）；江苏省自然科学基金（No.BK20160709）；南京农业大学校级SRT项目（No.1813A11）

• 李轶涵
• 南京农业大学, 资源与环境科学学院, 南京 210095

• 姜恬
• 南京农业大学, 资源与环境科学学院, 南京 210095

• 周旭
• 南京农业大学, 资源与环境科学学院, 南京 210095

• 赵旭蕾
• 南京农业大学, 资源与环境科学学院, 南京 210095

• 陆隽鹤
• 南京农业大学, 资源与环境科学学院, 南京 210095

• 季跃飞
• 南京农业大学, 资源与环境科学学院, 南京 210095

• 摘要：硫酸根自由基（SO₄^·-）高级氧化技术（SR-AOPs）是一种新型的原位化学氧化技术（ISCO），在水处理领域具有广阔的应用前景，可用于治理土壤和地下水中抗生素污染.本研究采用热活化过硫酸盐（PS）产生SO₄^·-，考察其对水溶液中抗生素卡巴多司（CBX）和奥喹多司（OQX）的降解效果，评估操作参数和水质成分对CBX降解的影响，并对CBX的降解产物进行鉴定.结果表明，与OQX相比，CBX更容易被热活化PS工艺氧化降解，这可能是因为CBX含有富电子的腙支链，而OQX含有惰性的酰胺支链.升高温度、增加PS浓度和降低溶液pH值均可显著促进CBX的降解.HCO₃^-的存在对CBX降解有促进作用，可能是由于生成的碳酸根自由基（CO₃^·-）参与了反应.Suwannee河富里酸（SRFA）具有双重影响，低浓度时促进CBX降解，而高浓度时呈现抑制作用.NO₃^-的存在对CBX的降解没有明显影响，而NO₂^-的存在可以显著抑制其降解.CBX在天然地表水中的降解效率低于在地下水中的效率，可能与不同水质中天然有机质的含量有关.产物鉴定表明，热活化PS氧化降解CBX生成了羟基化、脱氧和支链断裂产物，表明氧化反应主要改变了CBX分子中的腙支链和N-O结构.研究表明，热活化PS工艺可有效降解水溶液中的CBX和OQX，但在该技术实际应用时应充分评估天然水质成分的影响.

• Abstract：Sulfate radical (SO₄^·-)-based advanced oxidation processes (SR-AOPs) are promising in-situ chemical oxidation technologies (ISCO) that can be utilized for remediation of soil and groundwater contaminated by organic pollutants such as antimicrobial agents. This work reports the degradation of antimicrobial agents, i.e., carbadox (CBX) and olaquindox (OQX), in aqueous solution by SO₄^·- generated by thermally activated persulfate (PS) process. The effects of operational parameters and water constituents on the degradation of CBX were evaluated, and degradation products of CBX were identified. Experimental results show that CBX was more amenable toward oxidation by thermally activated PS process, presumably due to the electron-rich hydrazine side chain. Increasing temperature and PS dosage as well as decreasing solution pH enhanced the oxidation of CBX appreciably. The presence of bicarbonate (HCO₃^-) promoted the degradation of CBX, possible due to the involvement of carbonate radical (CO₃^·-). Suwannee river fulvic acid (SRFA) played a dual role as low concentration of SRFA promoted the degradation of CBX while high concentration inhibited the degradation. The presence of nitrate (NO₃^-) had no significant impact on CBX degradation; however, the presence of nitrite (NO₂^-) could remarkably inhibit the removal efficiency. The degradation efficiency of CBX in natural surface water was lower than that in ground water, possibly due to the difference in natural organic matter contents in water matrix. Degradation products of CBX, including hydroxylated, deoxygenated, and side chain cleaving products were identified, suggesting that oxidation mainly altered the structures of hydrazine chain and N-O moieties. Our contribution suggests that thermally activated PS process are effective for degradation of CBX and OQX; however, the impacts of natural water constituents should be carefully evaluated before using this technology for environmental remediation.

• Key words：carbadox  olaquindox  persulfate  sulfate radical  degradation

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