乙二胺修饰核壳磁性载金催化剂及其催化还原对硝基苯酚  

Ethylenediamine modified core-shell magnetic Au-supported nanocatalysts for reduction of 4-nitrophenol

作　　者：方嘉声 刁琪琪 陈铭 卫昆 邓楚昕 张国斐 FANG Jiasheng;DIAO Qiqi;CHEN Ming;WEI Kun;DENG Chuxin;ZHANG Guofei(School of Environment and Civil Engineering,Dongguan University of Technology,Dongguan 523808;Guangdong Xinchuang Huake Environmental Protection Co.,Ltd.,Dongguan 523000)

机构地区：[1]东莞理工学院生态环境与建筑工程学院,东莞523808 [2]广东新创华科环保股份有限公司,东莞523000

出　　处：《环境科学学报》2023年第5期228-237,共10页Acta Scientiae Circumstantiae

基　　金：国家自然科学基金项目(No.22008031);广东省基础与应用基础研究基金项目(No.2019A1515110426);东莞市科技特派员项目(No.20221800500622);东莞理工学院大学生创新创业训练计划项目(No.202111819064)。

摘　　要：采用Au(en)_(2)Cl_(3)化合物为介质的沉积沉淀法对制备的核壳梭型微球Fe_(2)O_(3)@MO_(2)(M:Ce、Ti或Si)进行乙二胺修饰并界面键合Au离子,通过两级连续还原气氛热处理,固载的Au离子首先还原为2~3 nm的纳米Au颗粒,Fe2O3转化为小体积Fe颗粒,并赋予核壳微球强磁性能,得到Fe@Au/MO_(2)催化剂.纳米Au颗粒在乙二胺为配体的稳定作用下封装固化于MO_(2)壳层结构,而壳层对Fe内核具有较好的保护作用.表征结果显示,Fe@Au/MO_(2)材料具有内空腔豌豆状核壳磁性结构及特定化学组成.该催化剂在温和条件下可将对硝基苯酚污染物进行还原性降解和资源转化,促进水体污染物化学资源综合利用.同时,研究了不同MO_(2)壳层结构对催化剂还原降解对硝基苯酚污染物的催化性能的影响.结果显示,Fe@Au/MO_(2)材料具有优异的磁分离性能和较好的循环使用性能,Fe@Au/CeO_(2)材料的催化反应性能最优.Core-shell spindle-like microspheres Fe_(2)O_(3)@MO_(2)(M:Ce,Ti or Si)were modified by ethylenediamine using Au(en)_(2)Cl_(3) compounds as the medium through the deposition and precipitation method,where the Au ions were immobilized at the interface.Via the two-stage continuous reduction atmosphere heat treatment,the Au ions were firstly reduced to 2~3 nm Au nanoparticles.Meanwhile,Fe2O3 cores were converted into small Fe particles,where core-shell composite microspheres were endowed with strong magnetic properties,and finally Fe@Au/MO_(2) catalysts were obtained.Au nanoparticles were encapsulated and solidified in MO_(2) shell structures under the stabilization of ethylenediamine as ligands,and theses shell structures had a good protective effect on Fe cores.The characterization results showed that Fe@Au/MO_(2) possessed prominent pea-like core-shell magnetic structures and specific chemical compositions.These catalysts can reductively degrade harmful 4-nitrophenol pollutant and convert it into useful resource under mild conditions,which would promote comprehensive utilization of chemical resources from aqueous pollutants.The influence of MO_(2) shell structures on the catalytic performance of reductive degradation of 4-nitrophenol were studied.The results show that Fe@Au/MO_(2) catalysts displayed excellent magnetic separation performance and good recycling ability,and the catalytic performance of Fe@Au/CeO_(2) material was the best.

关 键 词：核壳磁性结构 纳米Au颗粒 催化还原 对硝基苯酚 乙二胺 

分 类 号：X703[环境科学与工程—环境工程]