摘要
为了解决目前过硫酸盐活化材料稳定性差、重复使用性能欠佳的问题,本文使用二氧化硅气凝胶固定CoFe_(2)O_(4)纳米颗粒,合成了一种具有高比表面积的多孔CoFe_(2)O_(4)/二氧化硅气凝胶复合材料(SCF).采用扫描电子显微镜、透射电子显微镜、X射线衍射仪、X射线光电子能谱仪、电子顺磁共振波谱仪、傅里叶变换红外光谱仪和氮气吸附-脱附测试等手段对催化剂进行了表征.结果表明,二氧化硅气凝胶大大缓解了CoFe_(2)O_(4)纳米颗粒的团聚,CoFe_(2)O_(4)的负载在保留二氧化硅气凝胶高比表面积的同时,丰富了复合材料的孔隙结构.优化后的SCF在低负载(30%,质量分数)下,随着四环素(TC)浓度的上升,体系中的PMS分子消耗速率提高,降解效率逐渐降低.当TC浓度为25 mg/L时,去除率达到92.6%;当TC浓度50 mg/L时,在30 min的去除率依然超过80%,达到84.79%.通过猝灭实验确定SO_(4)^(∙-),1O^(2)和∙O_(4)^(-)为催化反应中主要的活性物质,并推测了可能的反应机理和降解途径.复合材料还表现出优异的稳定性和pH耐受性.
In this work,a porous CoFe_(2)O_(4)/silica aerogel gel composite(SCF)with a high specific surface area was successfully synthesized by using silica aerogel as a CoFe_(2)O_(4) carrier.The catalyst was systematically characterized by scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray diffraction analysis(XRD),X-ray photoelectron spectroscopy(XPS),electron paramagnetic resonance spectroscopy,Fourier transform infrared spectroscopy(FTIR),and nitrogen adsorption-desorption testing.The analysis shows that silica aerogel greatly alleviates the agglomeration of CoFe_(2)O_(4) nanoparticles,and the successful loading of CoFe_(2)O_(4) enriches the pore structure of the composite while retaining the high specific surface area of silica aerogel.The optimized SCF-30 achieved a removal efficiency of 84.79%for 50 mg/L TC solution after peroxymonosulfate(PMS)activation with low loading amount.Through quenching experiments,SO_(4)^(∙-),1O_(2),and∙O_(4)^(-) were identified as the main active substances in the catalytic reaction,and possible reaction mechanisms and degradation pathways were speculated.In addition,composite materials exhibit excellent stability and pH tolerance.This work provides insights into the design and fabrication of highly stable persulfate-activating materials.
作者
谭烨
周志宏
吴优
童海霞
喻林萍
曾巨澜
TAN Ye;ZHOU Zhihong;WU You;TONG Haixia;YU Linping;ZENG Julan(School of Chemistry and Pharmaceutical Engineering,Changsha University of Science&Technology,Changsha 410114,China;College of Energy and Power Engineering,Changsha University of Science&Technology,Changsha 410114,China)
出处
《高等学校化学学报》
北大核心
2025年第9期104-112,共9页
Chemical Journal of Chinese Universities
基金
国家自然科学基金(批准号:22073011,52074039)
湖南省自然科学基金(批准号:2017JJ1026,2025JJ60114)
湖南省教育厅科研项目(批准号:24A0217)资助。
关键词
氧化硅气凝胶
铁氧体
四环素
过硫酸盐
高级氧化技术
Silica aerogel
Ferrite
Tetracycline
Peroxymonosulfate
Advanced oxidation process
作者简介
联系人:曾巨澜,男,博士,教授,主要从事多孔材料合成及应用方面的研究.E-mail:jlzeng@csust.edu.cn。
