Electrochemical incineration of omeprazole in neutral aqueous medium using a platinum or boron-doped diamond anode

Degradation kinetics and oxidation products

Eliane Bezerra Cavalcanti, Sergio GARCIA SEGURA, Francesc Centellas, Enric Brillas

Research output: Contribution to journalArticle

89 Citations (Scopus)

Abstract

The electrochemical incineration of omeprazole, a widely prescribed gastrointestinal drug which is detected in natural waters, has been studied in a phosphate buffer of pH 7.0 by anodic oxidation with electrogenerated H2O2 (AO-H2O2) operating at constant current density (j). The experiments were carried out in a cell equipped with either a Pt or a boron-doped diamond (BDD) anode and an air-diffusion cathode to continuously produce H2O2. In these systems, organics are mainly oxidized by hydroxyl radicals formed at the Pt or BDD surface from water oxidation. A partial total organic carbon (TOC) abatement close to 78% for omeprazole was achieved by AO-H2O2 with a BDD anode after consumption of 18 Ah L-1 at 100 mA cm-2, whereas the alternative use of Pt did not allow mineralizing the drug. However, the drug was totally removed using both anodes, although it decayed more rapidly using BDD. In this latter system, increasing j accelerated the degradation process, but lowering the mineralization current efficiency. Greater drug content also enhanced the degradation rate with higher mineralization degree and current efficiency. The kinetics for omeprazole decay always followed a pseudo-first-order reaction and its rate constant increased with increasing j and with decreasing its concentration. Seven heteroaromatic intermediates and four hydroxylated derivatives were detected by LC-MS, while nine short-linear carboxylic acids were identified and quantified by ion-exclusion HPLC. These acids were largely accumulated using Pt and rapidly removed using BDD, thus explaining the partial mineralization of omeprazole achieved by AO-H2O2 with the latter anode. The release of inorganic ions such as NO3-, NH4+ and SO42- was followed by ionic chromatography. A plausible reaction sequence for omeprazole mineralization involving all intermediates detected is proposed.

Original languageEnglish (US)
Pages (from-to)1803-1815
Number of pages13
JournalWater Research
Volume47
Issue number5
DOIs
StatePublished - Apr 1 2013
Externally publishedYes

Fingerprint

Incineration
incineration
platinum
boron
diamond
Boron
Platinum
Diamonds
Anodes
Anodic oxidation
drug
oxidation
Degradation
kinetics
Oxidation
degradation
Kinetics
mineralization
ion
Ions

Keywords

  • Anodic oxidation
  • Degradation kinetics
  • Generated carboxylic acids
  • Heteroaromatic products
  • Omeprazole
  • Water treatment

ASJC Scopus subject areas

  • Water Science and Technology
  • Waste Management and Disposal
  • Pollution
  • Ecological Modeling

Cite this

Electrochemical incineration of omeprazole in neutral aqueous medium using a platinum or boron-doped diamond anode : Degradation kinetics and oxidation products. / Cavalcanti, Eliane Bezerra; GARCIA SEGURA, Sergio; Centellas, Francesc; Brillas, Enric.

In: Water Research, Vol. 47, No. 5, 01.04.2013, p. 1803-1815.

Research output: Contribution to journalArticle

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abstract = "The electrochemical incineration of omeprazole, a widely prescribed gastrointestinal drug which is detected in natural waters, has been studied in a phosphate buffer of pH 7.0 by anodic oxidation with electrogenerated H2O2 (AO-H2O2) operating at constant current density (j). The experiments were carried out in a cell equipped with either a Pt or a boron-doped diamond (BDD) anode and an air-diffusion cathode to continuously produce H2O2. In these systems, organics are mainly oxidized by hydroxyl radicals formed at the Pt or BDD surface from water oxidation. A partial total organic carbon (TOC) abatement close to 78{\%} for omeprazole was achieved by AO-H2O2 with a BDD anode after consumption of 18 Ah L-1 at 100 mA cm-2, whereas the alternative use of Pt did not allow mineralizing the drug. However, the drug was totally removed using both anodes, although it decayed more rapidly using BDD. In this latter system, increasing j accelerated the degradation process, but lowering the mineralization current efficiency. Greater drug content also enhanced the degradation rate with higher mineralization degree and current efficiency. The kinetics for omeprazole decay always followed a pseudo-first-order reaction and its rate constant increased with increasing j and with decreasing its concentration. Seven heteroaromatic intermediates and four hydroxylated derivatives were detected by LC-MS, while nine short-linear carboxylic acids were identified and quantified by ion-exclusion HPLC. These acids were largely accumulated using Pt and rapidly removed using BDD, thus explaining the partial mineralization of omeprazole achieved by AO-H2O2 with the latter anode. The release of inorganic ions such as NO3-, NH4+ and SO42- was followed by ionic chromatography. A plausible reaction sequence for omeprazole mineralization involving all intermediates detected is proposed.",
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