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. 2024 Apr 13;17(8):1791.
doi: 10.3390/ma17081791.

The Solvent Role for the Decomposition of Paracetamol in Distilled and Drinking Water by Pure and Ag-Modified TiO2 Sol-Gel Powders

Albena Bachvarova-Nedelcheva  1 , Reni Iordanova  1 , Nina Kaneva  2
Affiliations

The Solvent Role for the Decomposition of Paracetamol in Distilled and Drinking Water by Pure and Ag-Modified TiO2 Sol-Gel Powders

Albena Bachvarova-Nedelcheva et al. Materials (Basel). .

Abstract

In this study, pure TiO2 gels were synthesized by applying the sol-gel method, using Ti(IV) butoxide with the addition of two different solvents, namely ethylene glycol (EG) and isopropanol (isop), with only air moisture present. It was established using XRD that the gel prepared with the addition of EG was amorphous even at 400 °C, while the other gel was amorphous up to 300 °C. It was found that TiO2 (anatase) had a dominant crystalline phase during heating to 600 °C, while at 700 °C, TiO2 (rutile) appeared. The as-obtained powdered materials were annealed at 500 °C and subsequently underwent photocatalytic tests with paracetamol. Additionally, the TiO2 samples were modified with Ag+ co-catalysts (10-2 M), using photofixation by UV illumination. The photocatalytic activity of the Ag-modified powders was also tested in the photodegradation of a commonly used paracetamol in aqueous solution under UV light illumination. The obtained data exhibited that the annealed samples had better photocatalytic efficiency and decomposed paracetamol faster in comparison to the non-annealed sol-gel powders. The highest degradation efficiency was observed for the TBT/isop/Ag material, with degradation efficiencies average values of 65.59% and 75.61% paracetamol achieved after the third cycle of photocatalytic treatment. The co-catalytically modified powders had higher photocatalytic efficiency in comparison to the pure nanosized powders. Moreover, the sol-gel powders of TBT/EG, TBT/EG/Ag (10-2 M), TBT/isop, and TBT/isop/Ag (10-2 M) demonstrated the ability to retain their photocatalytic activity even after three cycles of use, suggesting that they could find practical use in the treatment of pharmaceutical wastewater. The observed photocatalytic efficiency and positive impact of silver make the prepared powders a desirable choice for pharmaceutical drug degradation, helping to promote environmentally friendly and effective wastewater treatment technology.

Keywords: Ag/TiO2 powders; distilled and drinking water; paracetamol; photocatalytic degradation; sol–gel.

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Conflict of interest statement

The authors declare no conflicts of interest.

Figures

Figure 1
Figure 1
XRD patterns of Ti(IV) n-butoxide dissolved in EG (Ti(IV) but/EG) (a); isopropanol (Ti(IV) but/isop) (b) heat-treated at different temperatures and after photocatalysis: (A) TiO2 anatase, (R) TiO2 rutile (c,d); crystalline phase weight content of the studied samples at 500 °C (e).
Figure 2
Figure 2
(a) SEM images at different magnifications of the Ti(IV) n-butoxide dissolved in isopropanol (Ti(IV) but/isop) heat-treated at 500 °C. (b) SEM images at different magnifications of the Ti(IV) n-butoxide dissolved in EG (Ti(IV) but/EG) heat-treated at 500 °C. SEM images of the used catalysts are shown as insert images.
Figure 3
Figure 3
IR spectra of Ti(IV) but/EG and Ti(IV) but/isop heat-treated at different temperatures. Ti(IV) but/EG (a) and Ti(IV) but/isop (b).
Figure 4
Figure 4
UV–visible spectra of Ti(IV) n-butoxide dissolved in EG (Ti(IV) but/EG) (a) and isopropanol (Ti(IV) but/isop) (b) gels heat-treated at 200 °C.
Figure 5
Figure 5
The time course of the decrease in the concentration for the mineralization of paracetamol using non-annealed (a) and annealed (b) pure and silver-photofixed TiO2 sol–gel powders (TBT/isop and TBT/EG). Kinetics of the photocatalytic decomposition of analgesic in distilled water (c,d) under UV light illumination are illustrated.
Figure 6
Figure 6
The likely mechanism of paracetamol degradation by pure and silver-photofixed titanium dioxide using ultraviolet illumination.
Figure 7
Figure 7
Decrease in the paracetamol concentration in drinking water versus time of UV light illumination with non-annealed and annealed pure and silver-photofixed TiO2 powders (a,b).
Figure 8
Figure 8
TOC analysis, measured at the end of the third cycle of photocatalytic reaction in (a) distilled water and (b) drinking water.
Figure 9
Figure 9
Photostability of TBT/EG and TBT/EG/Ag (a,b) and TBT/isop and TBT/isop/Ag (c,d) sol–gel powders on the decomposition of paracetamol in distilled and drinking water using UV illumination; surface morphology and integrity of the starting material (e).
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