摘要
为提升铁基金属有机框架(Fe-MOFs)对印染废水深度处理的效能,采用原位掺杂溶剂热技术制备了混合Fe(Ⅱ)/Fe(Ⅲ)价态MIL-53(Fe)(MV-MIL-53(Fe))催化剂。借助X射线粉末衍射仪、场发射扫描电镜、氮气吸附仪和吡啶吸附红外光谱仪等对MV-MIL-53(Fe)晶体结构、微观形貌、孔结构和表面酸位等本征结构进行了测试分析。选取对硝基苯酚(4-NP)作为印染废水模型污染物,以过氧乙酸(PAA)为氧源,研究了MV-MIL-53(Fe)催化PAA降解4-NP的性能和关键活性物种。结果表明:Fe(Ⅱ)的引入提高了MIL-53(Fe)表面Lewis酸位密度,为PAA催化活化提供了更丰富更高效的活性位点;MV-MIL-53(Fe)/PAA体系对4-NP的降解速率常数高达0.0521 min^(-1),分别是MV-MIL-53(Fe)/H_(2)O_(2)、MIL-53(Fe)/PAA和MIL-53(Fe)/H_(2)O_(2)体系的2.05、1.45和6.68倍,且MV-MIL-53(Fe)重复循环使用5次后仍保持良好的结构稳定性和催化降解性能;羟基自由基(·OH)是MV-MIL-53(Fe)催化PAA快速降解4-NP的关键活性物质。
In order to improve the advanced treatment efficiency of iron-based metal-organic frame-works(Fe-MOFs)for printing and dyeing wastewater,mixed-valence MIL-53(Fe)(MV-MIL-53(Fe))containing Fe(Ⅱ)and Fe(Ⅲ)was prepared by an in-situ doping solvothermal approach.The MV-MIL-53(Fe)was systematically characterized with X-ray diffraction,scanning electron microscopy,nitrogen adsorption equipment,and pyridine chemisorbed infrared spectroscopy.p-nitrophenol and peracetic acid(PAA)were selected as the model target and green oxidant respectively to study the degradation activity and major active species of MV-MIL-53(Fe).The results show that Fe(Ⅱ)dopant increased the Lewis acidity of MIL-53(Fe),thus offering more active sites for PAA activation.The 4-NP degradation kinetic rate constant of MV-MIL-53(Fe)/PAA system could reach to 0.0521 min^(-1),which was 2.05,1.45,and 6.68 times higher than MV-MIL-53(Fe)/H_(2)O_(2),MIL-53(Fe)/PAA,and MIL-53(Fe)/H_(2)O_(2)counterparts,respectively.After successive cycling for five runs,the MV-MIL-53(Fe)still exhibited good structure stability and catalysis activity for 4-NP degradation using PAA.Hydroxyl radicals were verified as the main reactive species converting from PAA for the rapid degradation of 4-NP.
作者
胡倩
杨涛语
朱斐超
吕汪洋
吴明华
余德游
HU Qian;YANG Taoyu;ZHU Feichao;Lü Wangyang;WU Minghua;YU Deyou(Engineering Research Center for Eco-Dyeing and Finishing of Textiles,Ministry of Education,Zhejiang Sci-Tech University,Hangzhou,Zhejiang 310018,China;Tongxiang Research Institute,Zhejiang Sci-Tech University,Jiaxing,Zhejiang 314500,China;Key Laboratory of Advanced Textile Materials&Manufacturing Technology,Ministry of Education,Zhejiang Sci-Tech University,Hangzhou,Zhejiang 310018,China;School of Materials Science&Engineering,Zhejiang Sci-Tech University,Hangzhou,Zhejiang 310018,China)
出处
《纺织学报》
EI
CAS
CSCD
北大核心
2022年第11期133-140,共8页
Journal of Textile Research
基金
国家自然科学基金项目(22106141)
中国博士后科学基金项目(2022M712827)
浙江理工大学桐乡研究院博士后基金资助项目(TYY202103)。
关键词
铁基金属有机框架
过氧乙酸
催化降解
对硝基苯酚
印染废水
iron-based metal-organic framework
peracetic acid
catalytic degradation
p-nitrophenol
dyeing and printing wastewater