Degradation and Mineralization of Carbamazepine Using an Electro-Fenton Reaction Catalyzed by Magnetite Nanoparticles Fixed on an Electrocatalytic Carbon Fiber Textile Cathode

被引:136
作者
Liu, Kai [1 ]
Yu, Joseph Che-Chin [1 ,2 ]
Dong, Heng [1 ]
Wu, Jeffrey C. S. [2 ]
Hoffmann, Michael R. [1 ]
机构
[1] CALTECH, Dept Environm Sci & Engn, Pasadena, CA 91126 USA
[2] Natl Taiwan Univ, Dept Chem Engn, Taipei 10617, Taiwan
关键词
ADVANCED OXIDATION; HYDROGEN-PEROXIDE; PHOTOCATALYTIC OXIDATION; OXYGEN REDUCTION; WATER; PHARMACEUTICALS; CONTAMINANTS; EFFICIENCY; KINETICS; DIOXIDE;
D O I
10.1021/acs.est.8b03916
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Pharmaceutical wastes are considered to be important pollutants even at low concentrations. In this regard, carbamazepine has received significant attention due to its negative effect on both ecosystem and human health. However, the need for acidic conditions severely hinders the use of conventional Fenton reagent reactions for the control and elimination of carbamazepine in wastewater effluents and drinking water influents. Herein, we report of the synthesis and use of flexible bifunctional nanoelectrocatalytic textile materials, Fe3O4-NP@CNF, for the effective degradation and complete mineralization of carbamazepine in water. The nonwoven porous structure of the composite binder-free Fe3O4-NP@CNF textile is used to generate H2O2 on the carbon nanofiber (CNF) substrate by O-2 reduction. In addition, center dot OH radical is generated on the surface of the bonded Fe3O4 nanoparticles (NPs) at low applied potentials (-0.345 V). The Fe3O4-NPs are covalently bonded to the CNF textile support with a high degree of dispersion throughout the fiber matrix. The dispersion of the nanosized catalysts results in a higher catalytic reactivity than existing electro-Fenton systems. For example, the newly synthesized Fe3O4-NPs system uses an Fe loading that is 2 orders of magnitude less than existing electro-Fenton systems, coupled with a current efficiency that is higher than electrolysis using a boron-doped diamond electrode. Our test results show that this process can remove carbamazepine with high pseudo-first-order rate constants (e.g., 6.85 h(-1) ) and minimal energy consumption (0.239 kW.h/g carbamazepine). This combination leads to an efficient and sustainable electro-Fenton process.
引用
收藏
页码:12667 / 12674
页数:8
相关论文
共 42 条
[1]   ALIGNED CARBON NANOTUBE ARRAYS FORMED BY CUTTING A POLYMER RESIN-NANOTUBE COMPOSITE [J].
AJAYAN, PM ;
STEPHAN, O ;
COLLIEX, C ;
TRAUTH, D .
SCIENCE, 1994, 265 (5176) :1212-1214
[2]   Occurrence and analysis of parabens in municipal sewage sludge from wastewater treatment plants in Madrid (Spain) [J].
Albero, Beatriz ;
Ana Perez, Rosa ;
Sanchez-Brunete, Consuelo ;
Luis Tadeo, Jose .
JOURNAL OF HAZARDOUS MATERIALS, 2012, 239 :48-55
[3]   CRITICAL-REVIEW OF RATE CONSTANTS FOR REACTIONS OF HYDRATED ELECTRONS, HYDROGEN-ATOMS AND HYDROXYL RADICALS (.OH/.O-) IN AQUEOUS-SOLUTION [J].
BUXTON, GV ;
GREENSTOCK, CL ;
HELMAN, WP ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (02) :513-886
[4]   Electrochemical technologies in wastewater treatment [J].
Chen, GH .
SEPARATION AND PURIFICATION TECHNOLOGY, 2004, 38 (01) :11-41
[5]   Nanostructured Catalysts for Organic Transformations [J].
Chng, Leng Leng ;
Erathodiyil, Nandanan ;
Ying, Jackie Y. .
ACCOUNTS OF CHEMICAL RESEARCH, 2013, 46 (08) :1825-1837
[6]   A VOLTAMMETRIC INVESTIGATION OF OXYGEN REDUCTION IN A TRICKLE BED CELL USING GRAPHITE CHIP AND RVC CATHODES [J].
DAVISON, JB ;
KACSIR, JM ;
PEERCELANDERS, PJ ;
JASINSKI, R .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1983, 130 (07) :1497-1501
[7]   Degradation of the antiepileptic drug carbamazepine upon different UV-based advanced oxidation processes in water [J].
Deng, Jing ;
Shao, Yisheng ;
Gao, Naiyun ;
Xia, Shengji ;
Tan, Chaoqun ;
Zhou, Shiqing ;
Hu, Xuhao .
CHEMICAL ENGINEERING JOURNAL, 2013, 222 :150-158
[8]   Electrochemical Advanced Oxidation of Carbamazepine on Boron-Doped Diamond Anodes. Influence of Operating Variables [J].
Dominguez, Joaquin R. ;
Gonzalez, T. ;
Palo, P. ;
Sanchez-Martin, J. .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2010, 49 (18) :8353-8359
[9]   PHOTOCATALYTIC OXIDATION OF SULFUR-DIOXIDE IN AQUEOUS SUSPENSIONS OF ALPHA-FE2O3 [J].
FAUST, BC ;
HOFFMANN, MR ;
BAHNEMANN, DW .
JOURNAL OF PHYSICAL CHEMISTRY, 1989, 93 (17) :6371-6381
[10]   Mesoporous Nitrogen-Doped Carbon for the Electrocatalytic Synthesis of Hydrogen Peroxide [J].
Fellinger, Tim-Patrick ;
Hasche, Frederic ;
Strasser, Peter ;
Antonietti, Markus .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (09) :4072-4075