Nano-architecture of MOF (ZIF-67)-based Co3O4 NPs@N-doped porous carbon polyhedral nanocomposites for oxidative degradation of antibiotic sulfamethoxazole from wastewater

被引:86
作者
Mohtasham, Hamed [1 ,2 ]
Rostami, Mojtaba [3 ]
Gholipour, Behnam [4 ]
Sorouri, Amir Mohammad [5 ]
Ehrlich, Hermann [6 ,7 ]
Ganjali, Mohmmad Reza [8 ]
Rostamnia, Sadegh [4 ]
Rahimi-Nasrabadi, Mehdi [1 ,6 ,9 ]
Salimi, Abdollah [2 ]
Luque, Rafael [10 ,11 ]
机构
[1] Baqiyatallah Univ Med Sci, Syst Biol & Poisonings Inst, Chem Injuries Res Ctr, Tehran, Iran
[2] Univ Kurdistan, Dept Chem, Sanandaj 6617715175, Iran
[3] Univ Tehran, Coll Sci, Sch Chem, Tehran, Iran
[4] Iran Univ Sci & Technol IUST, Dept Chem, Organ & Nano Grp ONG, POB 16846-13114, Tehran, Iran
[5] Islamic Azad Univ, Sci & Res Branch Tehran, Fac Vet Sci, Tehran, Iran
[6] TU Bergakad Freiberg, Inst Elect & Sensor Mat, D-09599 Freiberg, Germany
[7] Adam Mickiewicz Univ, Ctr Adv Technol, PL-61614 Poznan, Poland
[8] Univ Tehran, Coll Sci, Sch Chem, Ctr Excellence Electrochem, Tehran, Iran
[9] Baqiyatallah Univ Med Sci, Fac Pharm, Tehran, Iran
[10] Univ Cordoba, Dept Quim Organ, Campus Rabanales,Edificio Marie Curie C-3, Cordoba, Spain
[11] RUDN Univ, Peoples Friendship Univ Russia, 6 Miklukho Maklaya Str, Moscow 117198, Russia
关键词
N-doped porous carbon; Degradation; Sulfamethoxazole; ZIF-67; Peroxymonosulfate; METAL-ORGANIC FRAMEWORK; RADICAL GENERATION; PEROXYMONOSULFATE; ACTIVATION; EFFICIENT; COBALT; SUPERSTRUCTURES; THERMOLYSIS; PERFORMANCE; MECHANISM;
D O I
10.1016/j.chemosphere.2022.136625
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Co3O4 NPs in N-doped porous carbon (Co3O4 NPs@N-PC) materials were prepared by one-pot pyrolysis of a ZIF-67 powder under N-2 atmosphere and followed by oxidation under air atmosphere (200 degrees C) toward promotion catalytic activity and activation of peroxymonosulfate (PMS) to degradation sulfamethoxazole (SMZ). 2-methylimidazole was used as a nitrogen source and a competitive ligand for the synthesis of Co3O4 NPs@N-PC, which in addition to affecting nucleation and growth of the crystal, promotes the production of active Co-N sites. Co3O4 NPs@N-PC nano-architecture has high specific surface areas (250 m(2) g(-1)) and is a non-toxic, effective and stable PMS activator. The effect of operating parameters including SMZ concentration, catalyst dosage, temperature and pH in the presence of Co3O4 NPs@N-PC was investigated. The Co3O4 NPs@N-PC composite showed superior performance in activating PMS over a wide range of pH (2-10) and different temperatures so that complete degradation of SMZ (50 mu M, 100 mL) was achieved within 15 min. The role of Co2+/Co3+ redox system in the mechanism before and after PMS activation was determined using XPS analysis. Surface-generated radicals led to the degradation of SMZ, in which the SMZ degradation rate attained 0.21 min(-1) with the mineralization of 36.8%. The feasible degradation mechanism of SMZ was studied in the presence of different scavengers and it was revealed that the degradation reaction proceeds from the radical/non-radical pathway and in this process most of the SO4 center dot- and center dot OH radicals are dominant. The recoverability and reuse of Co3O4 NPs@N-PC were evaluated to confirm its stability and potential for SMZ degradation and it was observed that the catalyst maintains its catalytic power for at least 5 cycles.
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页数:14
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