MIL-100(Fe,Mn)衍生物活化过氧化氢降解水中尼泊金丁酯
DEGRADATION OF BUTYLPARABEN IN WATER BY ACTIVATION OF HYDROGEN PEROXIDE BY MIL-100(Fe,Mn)DERIVATIVES
苑宇杰 1林涛1
作者信息
摘要
为实现水中典型的药物类新污染物尼泊金丁酯(BPB)的氧化降解,通过构建过渡金属的活性位点以及调控材料的结构特性,利用水热法及煅烧法合成了 MIL-100(Fe,Mn)衍生物催化剂用于催化H2O2降解水中BPB.详细探究了催化剂投加量和水环境化学条件(如初始pH、温度、共存离子等)对MIL-100(Fe,Mn)衍生物催化体系降解水中BPB的影响,同时对反应体系中活性物种进行鉴定分析.结果表明:MIL-100(Fe,Mn)衍生物催化体系在较宽pH范围和不同溶液温度范围(10℃～40℃)内均表现出良好的催化性能,且适当提高催化剂投加量有助于活化H2O2氧化水中BPB,优选pH=7.0、298 K(25 ℃)反应条件下投加0.2 g/L催化剂,然后加入1 mmol/L的H2O2可实现反应15 min内氧化降解96％的BPB.另外,反应体系中引入HCO3-对BPB降解起明显的抑制作用,但不同浓度的NO3-和Cl-对水中BPB降解效果影响不大.MIL-100(Fe,Mn)衍生物催化剂通过Fe、Mn金属离子之间的协同作用,可促进H2O2分解产生·OH,进而快速氧化水中BPB.
Abstract
The MIL-100(Fe,Mn)derivative catalyst,with new established active sites and regulated structure,was synthesized by hydrothermal method and calcination method to activate H2O2 for the removal of the typical new pharmaceutical pollutants,butylparaben(BPB)in water.The effects of catalyst dosage and water environmental chemical conditions(such as initial pH,reaction temperature,co-existing ions,etc.)on the degradation of BPB in water by MIL-100(Fe,Mn)derivatives were detailly investigated,and the active species in the reaction system were also analyzed.The results showed that the MIL-100(Fe,Mn)derivative catalytic system showed good catalytic performance in a wide range of pH and solution temperature,and increasing the catalyst dosage was conducive to the activation of H2O2 oxidation of BPB in water.Preferably,96％of BPB could be oxidized within 15 min by the MIL-100(Fe,Mn)derivative catalytic system under the conditions of pH=7.0,298 K(25 ℃),0.2 g/L catalyst and 1 mmol/L H2O2.In addition,the introduction of HCO3-in the reaction system significantly inhibited the degradation of BPB,but different concentration of NO3 and Cl-had little effect on the degradation of BPB in water.The synergistic interaction between Fe/Mn metal ions on the surface of MIL-100(Fe,Mn)derivative catalyst could promote the decomposition of H2O2 to generate*OH,and then rapidly oxidize BPB in water.
关键词
金属有机骨架材料/非均相催化氧化/过氧化氢/尼泊金丁酯/金属氧化物Key words
MOFs/heterogeneous catalytic oxidation/H2O2/butylparaben(BPB)/metal oxide引用本文复制引用
基金项目
国家重点研发计划(2022YFC3203702)
出版年
2024
NETL
NSTL
万方数据