Fenton-like degradation of sulfamethoxazole using Fe-based magnetic nanoparticles embedded into mesoporous carbon hybrid as an efficient catalyst

被引:237
作者
Tang, Juntao [1 ]
Wang, Jianlong [1 ,2 ]
机构
[1] Tsinghua Univ, Collaborat Innovat Ctr Adv Nucl Energy Technol, INET, Beijing 100084, Peoples R China
[2] Tsinghua Univ, Beijing Key Lab Radioact Waste Treatment, INET, Beijing 100084, Peoples R China
基金
中国国家自然科学基金;
关键词
Fenton-like catalyst; MOFs-derived material; Fe-based nanoparticles; Mesoporous carbon; Sulfamethoxazole; METAL-ORGANIC FRAMEWORK; PERSONAL CARE PRODUCTS; WASTE-WATER; HYDROGEN-PEROXIDE; HETEROGENEOUS CATALYST; GRAPHENE OXIDE; IRON-OXIDE; OXIDATION; COMPOSITE; REMOVAL;
D O I
10.1016/j.cej.2018.06.169
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Fe-based magnetic nanoparticles (NPs) embedded into mesoporous carbon hybrid (Fe@MesoC) was successfully fabricated from Fe-based metal-organic framework (MIL-100(Fe)) through a pyrolysis method, which was for the first time proposed as a novel Fenton-like catalyst for the degradation of sulfamethoxazole (SMX). The catalytic activity of Fe@MesoC was systematically evaluated on the basis of several reaction parameters including initial pH, initial H2O2 concentration and temperature. Under the optimal conditions, the Fe@MesoC composite demonstrated a superior catalytic activity for decomposing SMX in the presence of H2O2, and it accomplished 100% SMX and 54.5% total organic carbon (TOC) conversion within 120 min. Such outstanding performance can be explained by the excellent enrichment ability of the outer mesoporous carbon matrix, the abundant active sites of the inner Fe-based NPs, as well as the possible synergistic effect between the two components. Moreover, the facile electrons transfer from Fe-0 to iron oxide in the inner Fe-based NPs could facilitate the reduction of Fe3+ to Fe2+ ( represents the iron species anchored to the surface of the catalyst) and further improve the generation of hydroxyl radicals. With the high structural stability and saturation magnetization, the Fe@MesoC composite can be easily recycled for three subsequent runs without significant activity loss. The possible catalytic mechanism and degradation pathways for SMX degradation induced by hydroxyl radicals in Fe@MesoC/H2O2 Fenton-like system were also tentatively proposed.
引用
收藏
页码:1085 / 1094
页数:10
相关论文
共 58 条
[1]   Iron terephthalate metal-organic framework: Revealing the effective activation of hydrogen peroxide for the degradation of organic dye under visible light irradiation [J].
Ai, Lunhong ;
Zhang, Caihong ;
Li, Lili ;
Jiang, Jing .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2014, 148 :191-200
[2]   Precisely controlled encapsulation of Fe3O4 nanoparticles in mesoporous carbon nanodisk using iron based MOF precursor for effective dye removal [J].
Angamuthu, M. ;
Satishkumar, G. ;
Landau, M. V. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2017, 251 :58-68
[3]   Highly stable Fe/γ-Al2O3 catalyst for catalytic wet peroxide oxidation [J].
Bautista, Patricia ;
Mohedano, Angel F. ;
Casas, Jose A. ;
Zazo, Juan A. ;
Rodriguez, Juan J. .
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY, 2011, 86 (04) :497-504
[4]   On the textural and crystalline properties of Fe-carbon xerogels. Application as Fenton-like catalysts in the oxidation of paracetamol by H2O2 [J].
Carrasco-Diaz, M. R. ;
Castillejos-Lopez, E. ;
Cerpa-Naranjo, A. ;
Rojas-Cervantes, M. L. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2017, 237 :282-293
[5]   Highly active heterogeneous Fenton-like systems based on Fe0/Fe3O4 composites prepared by controlled reduction of iron oxides [J].
Costa, Regina C. C. ;
Moura, Flavia C. C. ;
Ardisson, J. D. ;
Fabris, J. D. ;
Lago, R. M. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2008, 83 (1-2) :131-139
[6]   Mesoporous sulfur-modified iron oxide as an effective Fenton-like catalyst for degradation of bisphenol A [J].
Du, Jiangkun ;
Bao, Jianguo ;
Fu, Xiaoyan ;
Lu, Chenghang ;
Kim, Sang Hoon .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2016, 184 :132-141
[7]   Graphenes as Efficient Metal-Free Fenton Catalysts [J].
Espinosa, Juan C. ;
Navalon, Sergio ;
Primo, Ana ;
Moral, Monica ;
Fernandez Sanz, Javier ;
Alvaro, Mercedes ;
Garcia, Hermenegildo .
CHEMISTRY-A EUROPEAN JOURNAL, 2015, 21 (34) :11966-11971
[8]   Clay-supported nanoscale zero-valent iron composite materials for the remediation of contaminated aqueous solutions: A review [J].
Ezzatahmadi, Naeim ;
Ayoko, Godwin A. ;
Millar, Graeme J. ;
Speight, Robert ;
Yan, Cheng ;
Li, Jihong ;
Li, Shizhong ;
Zhu, Jianxi ;
Xi, Yunfei .
CHEMICAL ENGINEERING JOURNAL, 2017, 312 :336-350
[9]  
Ferey G., 2004, ANGEW CHEM, V116, P6456, DOI DOI 10.1002/ANGE.200460592
[10]   The Chemistry and Applications of Metal-Organic Frameworks [J].
Furukawa, Hiroyasu ;
Cordova, Kyle E. ;
O'Keeffe, Michael ;
Yaghi, Omar M. .
SCIENCE, 2013, 341 (6149) :974-+