摘要
传统均相芬顿工艺处理废水中的四环素存在需要外加H_(2)O_(2)消耗大量铁离子、pH适用范围窄以及产生大量铁污泥等问题。通过设计xCu(Fe)/Pd-In/TiO_(2)系列双功能催化剂,构建了H_(2)O_(2)直接合成-芬顿(类芬顿)反应耦合体系,实现了H_(2)O_(2)高效合成及原位活化降解废水中四环素。采用XRD、TEM和EPR等表征技术对催化剂的晶体结构和微观形貌进行了分析,探究了pH值、四环素溶液初始质量浓度、催化剂质量浓度和共存离子等工艺条件对催化剂四环素去除性能的影响。结果表明,在温度为25℃、pH值为7、四环素溶液初始质量浓度为30 mg/L、催化剂质量浓度为0.2 g/L和无共存离子的最适宜反应条件下反应90 min后,2Fe/Pd-In/TiO_(2)催化剂的四环素去除率最高(88.1%);在上述条件下,pH值为3时,1Cu/Pd-In/TiO_(2)催化剂的四环素去除率最高(80.3%)。xFe/Pd-In/TiO_(2)催化剂的四环素去除能力整体强于xCu/Pd-In/TiO_(2)催化剂,这主要是由于Fe在催化剂表面分散更加均匀,且催化剂粒径相对更小。自由基捕获实验和EPR分析结果表明,·O_(2)^(-)和·OH为氧化降解四环素的主要活性氧物种,其中·O_(2)^(-)起主导作用。
The traditional homogeneous Fenton process has some problems,such as requiring the addition of H_(2)O_(2)to consume a large amount of iron ions,the narrow pH application range and the generation of a large amount of iron sludge.Through designing a series of xCu(Fe)/Pd-In/TiO_(2)bifunctional catalysts,a coupling H_(2)O_(2)direct synthesis-Fenton(Fenton like)reaction system was constructed to achieve efficient synthesis of H_(2)O_(2),and in-situ activation degradation of tetracycline in wastewater.XRD,TEM and EPR characterization techniques were used to analyze the crystal structure and microscopic topography of the catalysts,and the effects of pH value,initial mass concentration of tetracycline solution,mass concentration of catalysts and coexisting ions on the tetracycline removal performances of the catalysts were investigated.The results show that the tetracycline removal rate of 2Fe/Pd-In/TiO_(2)catalyst is the highest(88.1%)after 90 min of reaction under the optimal reaction conditions of temperature of 25℃,pH value of 7,initial mass concentration of tetracycline solution of 30 mg/L,catalyst mass concentration of 0.2 g/L and no coexisting ions.Under the above conditions,the tetracycline removal rate of the 1Cu/Pd-In/TiO_(2)catalyst is the highest(80.3%)at pH value of 3.The tetracycline removal ability of xFe/Pd-In/TiO_(2)catalyst is better than that of xCu/Pd-In/TiO_(2)catalyst.This is mainly due to the more uniform dispersion of Fe on the catalyst surfaces and the relatively small particle size of the catalysts.The results of free radical capture experiment and EPR analysis show that·O_(2)^(-)and·OH are the main active oxygen species for oxidative degradation of tetracycline,in which·O_(2)^(-)plays a leading role.
作者
吕志文
宋文佳
苏敏
高嘉诚
贺嘉熙
欧阳李科
LV Zhiwen;SONG Wenjia;SU Min;GAO Jiacheng;HE Jiaxi;OUYANG Like(School of Chemical Engineering,Sichuan University,Chengdu 610207,Sichuan,China;Southwest Institute of Chemical Co.,Ltd.,Chengdu 610225,Sichuan,China)
出处
《低碳化学与化工》
CAS
北大核心
2024年第12期103-111,共9页
Low-Carbon Chemistry and Chemical Engineering
基金
国家自然科学基金青年基金(22008158)
四川省区域创新合作项目(2023YFQ0086)。
关键词
四环素去除
芬顿反应
活性氧物种
去除效率
tetracycline removal
Fenton reaction
active oxygen species
removal efficiency
