高等学校化学学报2024，Vol.45Issue(7)：145-155,11.DOI:10.7503/cjcu20240086
黄铁矿-Fe(Ⅲ)表面Lewis酸位点增强微囊藻毒素催化水解的机制
Mechanism of Hydrolysis of Microcystins Enhanced by Lewis Acid Sites on the Surface of Pyrite-Fe(Ⅲ)
摘要
Abstract
Natural mineral(Pyrite)can effectively degrade microcystins(Microcystins,MCs)in water at warm temperature(60℃)(k=0.072 min‒1),but how to break through the heat bottleneck and attain efficient degradation of MCs at room temperature[(25±5)℃]are still a technical issue in water treatment nowadays.In this study,the addition of iron ions(Fe3+,FeCl3)can accelerate the hydrolysis efficiency of microcystins-RR(Microcystin-RR,MC-RR)in pyrite system at room temperature(hydrolysis contribution rate 77.94%),and the degradation rate constant(0.36 h‒l)was three times higher than that of pyrite alone(0.12 h‒l).X-ray photoelectron spectroscopy(XPS),cyclic voltammetry(CV),in situ attenuated total reflection-Fourier transform infrared spectroscopy(in situ ATR-FTIR)and density functional theory(DFT)suggested that the addition of Fe3+enhanced the amount of iron sites of Lewis acid on pyrite surface by forming Fe(Ⅲ)—O bond,and then hydrolyzed MC-RR amide bond through its coordination with C=O.Additionally,the addition of Fe3+can oxidize the multivalent sulfur species on the surface of pyrite(Sn2 ‒,S22 ‒)to elemental sulfur(S0),further promoting the hydrolysis of MC-RR by forming hydrogen bond(—NH…S).This study not only provides a normal temperature mineral treatment technology for cyanobacteria bloom treatment,but also provides a theoretical basis for the self-purification mechanism of amide organic pollutants in natural water.关键词
微囊藻毒素/Lewis酸位点/水解/黄铁矿/催化机制Key words
Microcystins/Lewis acid site/Hydrolysis/Pyrite/Catalytic mechanism分类
化学引用本文复制引用
兰星,贺玉婷,张清,方艳芬,邓安平,赵海霞,张兆年..黄铁矿-Fe(Ⅲ)表面Lewis酸位点增强微囊藻毒素催化水解的机制[J].高等学校化学学报,2024,45(7):145-155,11.基金项目
国家自然科学基金(批准号:22076098,21577078,22376118)、湖北省自然科学基金杰出青年项目(批准号:2023AFA054)和地方高校能源和环境材料化学学科创新引智基地(批准号:D20015).Supported by the National Natural Science Foundation of China(Nos.22076098,22376118,21577078),the Outstanding Youth Project of the Natural Science Foundation of Hubei Province,China(No.2023AFA054)and the 111 Project of China(No.D20015). （批准号:22076098,21577078,22376118）
