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

Co3O4 NPs in N-doped porous carbon (Co3O4 NPs@N-PC) materials were prepared by one-pot pyrolysis of a ZIF-67 powder under N2 atmosphere and followed by oxidation under air atmosphere (200 °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 m2 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 μM, 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[rad]− and [rad]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. © 2022

Авторы
Mohtasham H. , Rostami M. , Gholipour B. , Sorouri A.M. , Ehrlich H. , Ganjali M.R. , Rostamnia S. , Rahimi-Nasrabadi M. , Salimi A. , Luque R.
Журнал
Издательство
Elsevier Ltd
Язык
Английский
Статус
Опубликовано
Номер
136625
Том
310
Год
2023
Организации
  • 1 Chemical Injuries Research Center, Systems Biology and Poisonings Institute, Baqiyatallah University of Medical Sciences, Tehran, Iran
  • 2 Department of Chemistry, University of Kurdistan, Sanandaj, 66177-15175, Iran
  • 3 School of Chemistry, College of Science, University of Tehran, Tehran, Iran
  • 4 Organic and Nano Group (ONG), Department of Chemistry, Iran University of Science and Technology (IUST), PO Box 16846-13114, Tehran, Iran
  • 5 Islamic Azad University, Science & Research Branch-Tehran, Faculty of Veterinary Science, Tehran, Iran
  • 6 Institute of Electronic and Sensor Materials, TU Bergakademie Freiberg, Freiberg, 09599, Germany
  • 7 Center for Advanced Technology, Adam Mickiewicz University, Poznan, 61614, Poland
  • 8 Center of Excellence in Electrochemistry, School of Chemistry, College of Science, University of Tehran, Tehran, Iran
  • 9 Faculty of Pharmacy, Baqiyatallah University of Medical Sciences, Tehran, Iran
  • 10 Departamento de Química Orgánica, Universidad de Córdoba, Campus de Rabanales, Edificio Marie Curie (C-3), Ctra Nnal IV-A, Km 396, Cordoba, E14014, Spain
  • 11 Peoples Friendship University of Russia (RUDN University), 6 Miklukho Maklaya str., Moscow, 117198, Russian Federation
Ключевые слова
Co<sub>3</sub>O<sub>4</sub> NPs; Degradation; N-doped porous carbon; Peroxymonosulfate; Sulfamethoxazole; ZIF-67
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