中文关键词Cu⁰@Fe₃O₄活化过一硫酸盐对-硝基苯酚(PNP)非均相反应协同修复 英文关键词Cu⁰@Fe₃O₄activate PMSp-nitrophenol(PNP)heterogeneous reactioncollaborative remediation

作者	单位	E-mail
石清清	成都理工大学生态环境学院, 成都 610059 成都理工大学国家环境保护水土污染协同控制与联合修复重点实验室, 成都 610059	18428383200@163.com
蒲生彦	成都理工大学生态环境学院, 成都 610059 成都理工大学国家环境保护水土污染协同控制与联合修复重点实验室, 成都 610059 中国环境科学研究院环境基准与风险评估国家重点实验室, 北京 100012	pushengyan@gmail.com
杨犀	成都理工大学生态环境学院, 成都 610059 成都理工大学国家环境保护水土污染协同控制与联合修复重点实验室, 成都 610059

中文摘要 为解决纳米Cu⁰活化过硫酸盐体系主要依赖浸出铜离子参与均相反应且适应pH范围窄（<7）的缺陷，本研究采用共沉淀法制备了纳米Cu⁰@Fe₃O₄催化剂，以对-硝基苯酚（PNP）为目标污染物，较系统地考察了Cu⁰@Fe₃O₄活化PMS的性能和降解PNP的反应机制.结果表明：① pH=5.65、200 mg ·L^-1 Cu⁰@Fe₃O₄和0.5 mmol ·L^-1 PMS在60 min内对5 mg ·L^-1 PNP的降解率可达到96%；②在Cu⁰@Fe₃O₄/PMS体系中，总铜离子（TCu）和总亚铜离子（TCu⁺）以及铁离子浸出几乎可以忽略，可认为是非均相反应体系；③通过包覆Fe₃O₄成功改变了Cu⁰活化PMS降解PNP的反应途径，在5~9的pH范围内都具有良好的降解性能；④反应体系中存在SO^-₄ ·和HO ·两种活性自由基，对反应体系的贡献率分别为34%和60%，HO ·是主导自由基；⑤体系中Fe和Cu之间存在双金属协同作用，Cu（Ⅰ）的存在能够促进Fe（Ⅲ）还原为Fe（Ⅱ），从而形成良好的氧化还原循环，提高了反应体系的持久性. 英文摘要 A Cu⁰/PMS system mainly relies on the leaching of copper ions to degrade the pollutants and adapt to the narrow pH range (<7). To solve this defect, we studied the properties and reaction mechanism of Cu⁰@Fe₃O₄ magnetic core-shell material, which was successfully prepared using co-precipitation method, taking PNP as the target pollutant. The results showed that: ① a degradation rate of 96% can be achieved within 60 min for 5 mg ·L^-1 PNP, 200 mg ·L^-1 Cu⁰@Fe₃O₄, and 0.5 mmol ·L^-1 PMS at a natural pH value (5.65); ② the Cu⁰@Fe₃O₄/PMS system can be regarded as a heterogeneous reaction system because TCu, TCu⁺, and iron leaching were almost negligible; ③ on comparing the performance of the Cu⁰@Fe₃O₄/PMS system and Cu⁰/PMS system in the pH range of 3 to 11, it was discovered that the method by which Cu⁰ activates the PMS to degrade the PNP was successfully changed by coating a layer of Fe₃O₄. The Cu⁰@Fe₃O₄/PMS system has a good degradation performance towards PNP in the pH range of 5-9; ④ SO^-₄ · and HO · existed in the reaction system, and their contribution rates to the reaction system were 34% and 60% ; HO · was the dominant free radical; ⑤ A bimetallic synergy exists between Fe and Cu. The presence of Cu(Ⅰ) can promote the reduction of Fe(Ⅲ) to Fe(Ⅱ), thereby forming a good redox cycle and improving the durability of the reaction system.

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