Abstract

The presence of pharmaceuticals in surface water, drinking water, and wastewater has attracted significant concern because of the non-biodegradability, resistance, and toxicity of pharmaceutical compounds. The catalytic ozonation of an anti-inflammatory pharmaceutical, ibuprofen was investigated in this work. The reaction mixture was analyzed and measured by high-performance liquid chromatography (HPLC). Liquid chromatography-mass spectrometry (LC-MS) was used for the quantification of by-products during the catalytic ozonation process. Ibuprofen was degraded by ozonation under optimized conditions within 1 h. However, some intermediate oxidation products were detected during the ibuprofen ozonation process that were more resistant than the parent compound. To optimize the process, nine heterogeneous catalysts were synthesized using different preparation methods and used with ozone to degrade the ibuprofen dissolved in aqueous solution. The aim of using several catalysts was to reveal the effect of various catalyst preparation methods on the degradation of ibuprofen as well as the formation and elimination of by-products. Furthermore, the goal was to reveal the influence of various support structures and different metals such as Pd-, Fe-, Ni-, metal particle size, and metal dispersion in ozone degradation. Most of the catalysts improved the elimination kinetics of the by-products. Among these catalysts, Cu-H-Beta-150-DP synthesized by the deposition–precipitation process showed the highest decomposition rate. The regenerated Cu-H-Beta-150-DP catalyst preserved the catalytic activity to that of the fresh catalyst. The catalyst characterization methods applied in this work included nitrogen adsorption–desorption, scanning electron microscopy, transmission electron microscopy, and Fourier-transform infrared spectroscopy. The large pore volume and small metal particle size contributed to the improved catalytic activity.

Highlights

  • Due to a globally increasing consumption of pharmaceuticals in the recent years, a pharmaceutical cocktail has emerged in surface waters and effluents from human communities

  • IBU was determined via an high-performance liquid chromatography (HPLC) (Agilent Technologies 1100 series) with a UV-Vis photo diode array detector set at 214 nm, and a quaternary pump

  • The method of introduction of Cu- in H-Beta zeolite, the particle size of Cu, and acid sites were observed to influence the degradation of ibuprofen

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Summary

Introduction

Due to a globally increasing consumption of pharmaceuticals in the recent years, a pharmaceutical cocktail has emerged in surface waters and effluents from human communities. It is known that chlorine applied for the disinfection of drinking water is able to react with organic contaminates present in water and generate by-products such as chloroform This has directed to employ alternative disinfection processes such as catalytic ozonation [16]. Xin et al studied the CuO/SBA-15 catalyst preparation through the deposition–precipitation process This method displayed an effective and scalable way of fabricating a copper-based catalyst with a desirable oxidation activity [21]. The present work was designed to achieve the total decomposition of IBU and transformation products of IBU in a shorter time of ozonation For this purpose, different nitrogen concentrations were used in the inlet gas of ozonator, and nine different catalysts (Cu-H-Beta-25-IE, Cu-H-Beta-150-IE, Cu-H-Beta-300, Cu-H-Beta-150-EIM, Cu-H-Beta-150-DP, Cu-Na-Mordenite-12.8-IE, Pd-H-MCM-41-EIM, Fe-SiO2 -DP, and Ni-H-Beta-25-EIM) were used for the removal of IBU.

Physico-Chemical Characterization
Nitrogen Physisorption
Specific
Pyridine Adsorption–Desorption with FTIR Spectroscopy
Effect of Different Nitrogen Gas Flow Rate on the Decomposition of IBU
Quantification of Oxidation Products
10. The degradationofofIBU
Chemicals
Physico-Chemical Characterization of Employed Catalyst
Experiment Method for Ozonation Activity and Kinetics
Chemical Analysis
Conclusions

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