Radical induced degradation of acetaminophen with Fe3O4 magnetic nanoparticles as heterogeneous activator of peroxymonosulfate

Chaoqun Tan, Naiyun Gao, Yang Deng, Jing Deng, Shiqing Zhou, Jun Li, Xiaoyan Xin

Research output: Contribution to journalArticleResearchpeer-review

149 Citations (Scopus)

Abstract

Magnetic nano-scaled particles Fe3O4 were studied for the activation of peroxymonosulfate (PMS) to generate active radicals for degradation of acetaminophen (APAP) in water. The Fe3O4 MNPs were found to effectively catalyze PMS for removal of APAP, and the reactions well followed a pseudo-first-order kinetics pattern (R2>0.95). Within 120min, approximately 75% of 10ppm APAP was accomplished by 0.2mM PMS in the presence of 0.8g/L Fe3O4 MNPs with little Fe3+ leaching (<4μg/L). Higher Fe3O4 MNP dose, lower initial APAP concentration, neutral pH, and higher reaction temperature favored the APAP degradation. The production of sulfate radicals and hydroxyl radicals was validated through two ways: (1) indirectly from the scavenging tests with scavenging agents, tert-butyl alcohol (TBA) and ethanol (EtOH); (2) directly from the electron paramagnetic resonance (ESR) tests with 0.1M 5,5-dimethyl-1-pyrrolidine N-oxide (DMPO). Plausible mechanisms on the radical generation from Fe3O4 MNP activation of PMS are proposed based on the results of radical identification tests and XPS analysis. It appeared that Fe2+Fe3+ on the catalyst surface was responsible for the radical generation. The results demonstrated that Fe3O4 MNPs activated PMS is a promising technology for water pollution caused by contaminants such as pharmaceuticals.

Original languageEnglish
Pages (from-to)452-460
Number of pages9
JournalJournal of Hazardous Materials
Volume276
DOIs
StatePublished - 15 Jul 2014

Fingerprint

Scavenging
Acetaminophen
Nanoparticles
Paramagnetic resonance
Chemical activation
Degradation
degradation
Water pollution
Drug products
Leaching
electron spin resonance
Alcohols
Ethanol
X ray photoelectron spectroscopy
Impurities
Catalysts
Kinetics
Oxides
tert-Butyl Alcohol
Water Pollution

Keywords

  • Acetaminophen
  • Heterogeneous catalyst
  • Peroxymonosulfate
  • Radicals

Cite this

Tan, Chaoqun ; Gao, Naiyun ; Deng, Yang ; Deng, Jing ; Zhou, Shiqing ; Li, Jun ; Xin, Xiaoyan. / Radical induced degradation of acetaminophen with Fe3O4 magnetic nanoparticles as heterogeneous activator of peroxymonosulfate. In: Journal of Hazardous Materials. 2014 ; Vol. 276. pp. 452-460.
@article{a60d22cf96a54b70b97b657febbc65c5,
title = "Radical induced degradation of acetaminophen with Fe3O4 magnetic nanoparticles as heterogeneous activator of peroxymonosulfate",
abstract = "Magnetic nano-scaled particles Fe3O4 were studied for the activation of peroxymonosulfate (PMS) to generate active radicals for degradation of acetaminophen (APAP) in water. The Fe3O4 MNPs were found to effectively catalyze PMS for removal of APAP, and the reactions well followed a pseudo-first-order kinetics pattern (R2>0.95). Within 120min, approximately 75{\%} of 10ppm APAP was accomplished by 0.2mM PMS in the presence of 0.8g/L Fe3O4 MNPs with little Fe3+ leaching (<4μg/L). Higher Fe3O4 MNP dose, lower initial APAP concentration, neutral pH, and higher reaction temperature favored the APAP degradation. The production of sulfate radicals and hydroxyl radicals was validated through two ways: (1) indirectly from the scavenging tests with scavenging agents, tert-butyl alcohol (TBA) and ethanol (EtOH); (2) directly from the electron paramagnetic resonance (ESR) tests with 0.1M 5,5-dimethyl-1-pyrrolidine N-oxide (DMPO). Plausible mechanisms on the radical generation from Fe3O4 MNP activation of PMS are proposed based on the results of radical identification tests and XPS analysis. It appeared that Fe2+Fe3+ on the catalyst surface was responsible for the radical generation. The results demonstrated that Fe3O4 MNPs activated PMS is a promising technology for water pollution caused by contaminants such as pharmaceuticals.",
keywords = "Acetaminophen, Heterogeneous catalyst, Peroxymonosulfate, Radicals",
author = "Chaoqun Tan and Naiyun Gao and Yang Deng and Jing Deng and Shiqing Zhou and Jun Li and Xiaoyan Xin",
year = "2014",
month = "7",
day = "15",
doi = "10.1016/j.jhazmat.2014.05.068",
language = "English",
volume = "276",
pages = "452--460",
journal = "Journal of Hazardous Materials",
issn = "0304-3894",
publisher = "Elsevier",

}

Radical induced degradation of acetaminophen with Fe3O4 magnetic nanoparticles as heterogeneous activator of peroxymonosulfate. / Tan, Chaoqun; Gao, Naiyun; Deng, Yang; Deng, Jing; Zhou, Shiqing; Li, Jun; Xin, Xiaoyan.

In: Journal of Hazardous Materials, Vol. 276, 15.07.2014, p. 452-460.

Research output: Contribution to journalArticleResearchpeer-review

TY - JOUR

T1 - Radical induced degradation of acetaminophen with Fe3O4 magnetic nanoparticles as heterogeneous activator of peroxymonosulfate

AU - Tan, Chaoqun

AU - Gao, Naiyun

AU - Deng, Yang

AU - Deng, Jing

AU - Zhou, Shiqing

AU - Li, Jun

AU - Xin, Xiaoyan

PY - 2014/7/15

Y1 - 2014/7/15

N2 - Magnetic nano-scaled particles Fe3O4 were studied for the activation of peroxymonosulfate (PMS) to generate active radicals for degradation of acetaminophen (APAP) in water. The Fe3O4 MNPs were found to effectively catalyze PMS for removal of APAP, and the reactions well followed a pseudo-first-order kinetics pattern (R2>0.95). Within 120min, approximately 75% of 10ppm APAP was accomplished by 0.2mM PMS in the presence of 0.8g/L Fe3O4 MNPs with little Fe3+ leaching (<4μg/L). Higher Fe3O4 MNP dose, lower initial APAP concentration, neutral pH, and higher reaction temperature favored the APAP degradation. The production of sulfate radicals and hydroxyl radicals was validated through two ways: (1) indirectly from the scavenging tests with scavenging agents, tert-butyl alcohol (TBA) and ethanol (EtOH); (2) directly from the electron paramagnetic resonance (ESR) tests with 0.1M 5,5-dimethyl-1-pyrrolidine N-oxide (DMPO). Plausible mechanisms on the radical generation from Fe3O4 MNP activation of PMS are proposed based on the results of radical identification tests and XPS analysis. It appeared that Fe2+Fe3+ on the catalyst surface was responsible for the radical generation. The results demonstrated that Fe3O4 MNPs activated PMS is a promising technology for water pollution caused by contaminants such as pharmaceuticals.

AB - Magnetic nano-scaled particles Fe3O4 were studied for the activation of peroxymonosulfate (PMS) to generate active radicals for degradation of acetaminophen (APAP) in water. The Fe3O4 MNPs were found to effectively catalyze PMS for removal of APAP, and the reactions well followed a pseudo-first-order kinetics pattern (R2>0.95). Within 120min, approximately 75% of 10ppm APAP was accomplished by 0.2mM PMS in the presence of 0.8g/L Fe3O4 MNPs with little Fe3+ leaching (<4μg/L). Higher Fe3O4 MNP dose, lower initial APAP concentration, neutral pH, and higher reaction temperature favored the APAP degradation. The production of sulfate radicals and hydroxyl radicals was validated through two ways: (1) indirectly from the scavenging tests with scavenging agents, tert-butyl alcohol (TBA) and ethanol (EtOH); (2) directly from the electron paramagnetic resonance (ESR) tests with 0.1M 5,5-dimethyl-1-pyrrolidine N-oxide (DMPO). Plausible mechanisms on the radical generation from Fe3O4 MNP activation of PMS are proposed based on the results of radical identification tests and XPS analysis. It appeared that Fe2+Fe3+ on the catalyst surface was responsible for the radical generation. The results demonstrated that Fe3O4 MNPs activated PMS is a promising technology for water pollution caused by contaminants such as pharmaceuticals.

KW - Acetaminophen

KW - Heterogeneous catalyst

KW - Peroxymonosulfate

KW - Radicals

UR - http://www.scopus.com/inward/record.url?scp=84902260238&partnerID=8YFLogxK

U2 - 10.1016/j.jhazmat.2014.05.068

DO - 10.1016/j.jhazmat.2014.05.068

M3 - Article

VL - 276

SP - 452

EP - 460

JO - Journal of Hazardous Materials

JF - Journal of Hazardous Materials

SN - 0304-3894

ER -