Direct and indirect electrochemical oxidation of amine-containing pharmaceuticals using graphite electrodes

Yu Jung Liu, Ching Yao Hu, Shang Lien Lo

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

This study investigated the direct and indirect electro-oxidation of amine-containing pharmaceuticals (acetaminophen (ACT), diclofenac (DIC), and sulfamethoxazole (SMX)) by using graphite electrodes, and to compare the influence by using different electrolytes (Na2SO4 and NaCl). Under the optimum conditions of current (I) at 0.5 A, in direct system, 74.3%, 90.0%, 81.6% of ACT, DIC, and SMX were respectively removed after 60 min (k = 0.023, 0.037, 0.027 min−1), 48.9%, 85.9%, 68.2% of TOC respectively removed after reaction time. In contrast, at the same current intensity, in indirect system, ACT, DIC, and SMX were eliminated within 30 min (k = 0.117, 0.307, 0.170 min−1), 89.6%, 92.6%, 99.6% of TOC respectively removed after reaction time. The results indicated that the dissociated compounds were attracted to the anode due to electrostatic forces and had higher mass transformation rates in the direct electro-oxidation process. According to the cyclic voltammogram, indirect oxidation occurred when active chlorine species were generated from chloride ions anodically to destroy pollutants. Based on intermediates detected during electro-oxidation treatment by ultra performance liquid chromatography-quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS), only oxidized intermediates were found in the direct oxidation system, while both oxidized and chlorinated intermediates were found in the indirect oxidation system.

Original languageEnglish
Pages (from-to)592-605
Number of pages14
JournalJournal of Hazardous Materials
Volume366
DOIs
Publication statusPublished - Mar 15 2019

Fingerprint

Sulfamethoxazole
Graphite electrodes
Graphite
Electrooxidation
Diclofenac
Electrochemical oxidation
Acetaminophen
graphite
Drug products
Amines
Electrodes
electrode
drug
oxidation
Oxidation
Pharmaceutical Preparations
Electrostatic force
Chlorine
Liquid chromatography
Static Electricity

Keywords

  • Acetaminophen
  • Diclofenac
  • Direct oxidation
  • Indirect oxidation
  • Sulfamethoxazole

ASJC Scopus subject areas

  • Environmental Engineering
  • Environmental Chemistry
  • Waste Management and Disposal
  • Pollution
  • Health, Toxicology and Mutagenesis

Cite this

Direct and indirect electrochemical oxidation of amine-containing pharmaceuticals using graphite electrodes. / Liu, Yu Jung; Hu, Ching Yao; Lo, Shang Lien.

In: Journal of Hazardous Materials, Vol. 366, 15.03.2019, p. 592-605.

Research output: Contribution to journalArticle

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abstract = "This study investigated the direct and indirect electro-oxidation of amine-containing pharmaceuticals (acetaminophen (ACT), diclofenac (DIC), and sulfamethoxazole (SMX)) by using graphite electrodes, and to compare the influence by using different electrolytes (Na2SO4 and NaCl). Under the optimum conditions of current (I) at 0.5 A, in direct system, 74.3{\%}, 90.0{\%}, 81.6{\%} of ACT, DIC, and SMX were respectively removed after 60 min (k = 0.023, 0.037, 0.027 min−1), 48.9{\%}, 85.9{\%}, 68.2{\%} of TOC respectively removed after reaction time. In contrast, at the same current intensity, in indirect system, ACT, DIC, and SMX were eliminated within 30 min (k = 0.117, 0.307, 0.170 min−1), 89.6{\%}, 92.6{\%}, 99.6{\%} of TOC respectively removed after reaction time. The results indicated that the dissociated compounds were attracted to the anode due to electrostatic forces and had higher mass transformation rates in the direct electro-oxidation process. According to the cyclic voltammogram, indirect oxidation occurred when active chlorine species were generated from chloride ions anodically to destroy pollutants. Based on intermediates detected during electro-oxidation treatment by ultra performance liquid chromatography-quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS), only oxidized intermediates were found in the direct oxidation system, while both oxidized and chlorinated intermediates were found in the indirect oxidation system.",
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N2 - This study investigated the direct and indirect electro-oxidation of amine-containing pharmaceuticals (acetaminophen (ACT), diclofenac (DIC), and sulfamethoxazole (SMX)) by using graphite electrodes, and to compare the influence by using different electrolytes (Na2SO4 and NaCl). Under the optimum conditions of current (I) at 0.5 A, in direct system, 74.3%, 90.0%, 81.6% of ACT, DIC, and SMX were respectively removed after 60 min (k = 0.023, 0.037, 0.027 min−1), 48.9%, 85.9%, 68.2% of TOC respectively removed after reaction time. In contrast, at the same current intensity, in indirect system, ACT, DIC, and SMX were eliminated within 30 min (k = 0.117, 0.307, 0.170 min−1), 89.6%, 92.6%, 99.6% of TOC respectively removed after reaction time. The results indicated that the dissociated compounds were attracted to the anode due to electrostatic forces and had higher mass transformation rates in the direct electro-oxidation process. According to the cyclic voltammogram, indirect oxidation occurred when active chlorine species were generated from chloride ions anodically to destroy pollutants. Based on intermediates detected during electro-oxidation treatment by ultra performance liquid chromatography-quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS), only oxidized intermediates were found in the direct oxidation system, while both oxidized and chlorinated intermediates were found in the indirect oxidation system.

AB - This study investigated the direct and indirect electro-oxidation of amine-containing pharmaceuticals (acetaminophen (ACT), diclofenac (DIC), and sulfamethoxazole (SMX)) by using graphite electrodes, and to compare the influence by using different electrolytes (Na2SO4 and NaCl). Under the optimum conditions of current (I) at 0.5 A, in direct system, 74.3%, 90.0%, 81.6% of ACT, DIC, and SMX were respectively removed after 60 min (k = 0.023, 0.037, 0.027 min−1), 48.9%, 85.9%, 68.2% of TOC respectively removed after reaction time. In contrast, at the same current intensity, in indirect system, ACT, DIC, and SMX were eliminated within 30 min (k = 0.117, 0.307, 0.170 min−1), 89.6%, 92.6%, 99.6% of TOC respectively removed after reaction time. The results indicated that the dissociated compounds were attracted to the anode due to electrostatic forces and had higher mass transformation rates in the direct electro-oxidation process. According to the cyclic voltammogram, indirect oxidation occurred when active chlorine species were generated from chloride ions anodically to destroy pollutants. Based on intermediates detected during electro-oxidation treatment by ultra performance liquid chromatography-quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS), only oxidized intermediates were found in the direct oxidation system, while both oxidized and chlorinated intermediates were found in the indirect oxidation system.

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