纳米片形MFI-Fe分子筛活化H_(2)O_(2)降解酸性红G  

Degradation of Acidic Red G by H_(2)O_(2) Activated with Nanosheet MFI-Fe Zeolite

作　　者：许飞亚 姬亚军 杨鸿辉[3] 李清飞 张宗文 郭沛音 刘明华 XU Feiya;JI Yajun;YANG Honghui;LI Qingfei;ZHANG Zongwen;GUO Peiyin;LIU Minghua(Analysis&Testing Center,Xinyang Normal University,Xinyang 464000,Henan,China;Henan Key Laboratory for Synergistic Prevention of Water and Soil Environmental Pollution/School of Geographic Sciences,Xinyang Normal University,Xinyang 464000,Henan,China;School of Chemistry,Xi'an Jiaotong University,Xi'an 710049,China)

机构地区：[1]信阳师范大学分析测试中心,河南信阳464000 [2]信阳师范大学地理科学学院/河南省水土环境污染协同防治重点实验室,河南信阳464000 [3]西安交通大学化学学院,西安710049

出　　处：《硅酸盐学报》2024年第11期3492-3501,共10页Journal of The Chinese Ceramic Society

基　　金：国家自然科学基金(41671476);河南省科技攻关项目(242102320078);河南省高等学校重点科研项目(21A610010);信阳师范大学“南湖学者奖励计划”青年项目;信阳师范大学青年科研基金项目(2024-QN-043);河南省水土环境污染协同防治重点实验室开放基金(KLSPWSEP-A05)。

摘　　要：传统类芬顿催化剂在酸性条件下易溶出Fe导致活性下降。通过合成纳米片形MFI-Fe分子筛,将Fe镶嵌在分子筛骨架中,抑制Fe溶出,使其保持稳定的催化活性。结果表明:MFI-Fe通过活化H_(2)O_(2)产生HO·使酸性红G(ARG)降解。在pH=3、25℃、0.40 g/L MFI-Fe、20 mmol/L H_(2)O_(2)、180 min条件下,ARG(20 mg/L)的去除率达到约98.40%。溶液中NO_(3)^(-)、Cl^(-)、SO_(4)^(2-)共存离子对ARG的去除无影响,腐殖酸(HA)会轻微抑制ARG的降解。HCO_(3)^(-)会使溶液pH值升高,并消耗HO·导致ARG的去除率显著下降。反复使用5次MFI-Fe,Fe浸出量均小于0.42 mg/L,ARG的去除率保持在87.64%以上。Introduction The easy dissolution of Fe under acidic conditions results in the decreased activity of traditional Fenton-like catalysts.It was reported that the encapsulated or framework stabilized Fe-based materials showed excellent stability.Zeolite is a crystalline silicate/aluminosilicate with a stable framework structure,high specific surface area,uniform microporous and mesoporous structure,good acid-base resistance property.These characteristics make it a promising carrier or main material for Fenton-like catalysts.Therefore,a Fe-doped nanosheet MFI(MFI-Fe)zeolite was synthesized in this study.The Fe sites was embedded in the framework of MFI-Fe zeolite to inhibit the dissolution of Fe under acidic conditions,which could improve the performance of MFI-Fe zeolite for activating H_(2)O_(2)towards acidic red G(ARG)degradation in water.Methods With the assistance of diquaternary ammonium-type structural directing agents,the solid products were obtained through hydrothermal reactions(160℃,5 d)using tetraethyl orthosilicate and ferric chloride as the main raw materials.Then,MFI-Fe zeolite was obtained by calcining the solid products in air at 550℃for 3 h.X-ray diffraction spectroscopy(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),fourier transform infrared spectroscopy(FTIR),N_(2)adsorption-desorption and X-ray photoelectron spectroscopy(XPS)were applied to determine the physicochemical properties of MFI-Fe zeolite.The prepared MFI-Fe zeolite was applied to active H_(2)O_(2)for ARG degradation.The effects of catalyst dosage,H_(2)O_(2)dosage,solution pH value,reaction temperature,ARG concentration and coexisting ions on the degradation of ARG were studied.The concentration of ARG in the water was determined by an ultraviolet and visible(UV-Vis)spectrophotometer.Results and discussion According to the XRD and FTIR results,the prepared MFI-Fe zeolite exhibited the characteristic peaks of MFI zeolite,and there were not impurity peaks of silicon oxide or iron oxide,indicating that bo

关 键 词：MFI分子筛 类芬顿反应 酸性红G 降解 

分 类 号：X703[环境科学与工程—环境工程]