Efficient oxidation/mineralization of pharmaceutical pollutants using a novel Iron (III) oxyhydroxide nanostructure prepared via plasma technology: Experimental, modeling and DFT studies

Rasool Pelalak; Zahra Heidari; Reza Alizadeh; Eslam Ghareshabani; Negin Nasseh; Azam Marjani; Ahmad B Albadarin; Saeed Shirazian

doi:10.1016/j.jhazmat.2021.125074

Efficient oxidation/mineralization of pharmaceutical pollutants using a novel Iron (III) oxyhydroxide nanostructure prepared via plasma technology: Experimental, modeling and DFT studies

J Hazard Mater. 2021 Jun 5:411:125074. doi: 10.1016/j.jhazmat.2021.125074. Epub 2021 Jan 7.

Authors

Rasool Pelalak¹, Zahra Heidari², Reza Alizadeh², Eslam Ghareshabani³, Negin Nasseh⁴, Azam Marjani⁵, Ahmad B Albadarin⁶, Saeed Shirazian⁷

Affiliations

¹ Institute of Research and Development, Duy Tan University, Da Nang 550000, Viet Nam; Faculty of Environmental and Chemical Engineering, Duy Tan University, Da Nang 550000, Viet Nam.
² Chemical Engineering Faculty, Sahand University of Technology, Sahand New Town, Tabriz 51335-1996, Iran.
³ Physics Faculty, Sahand University of Technology, Sahand New Town, Tabriz 51335-1996, Iran.
⁴ Social Determinants of Health Research Center, Faculty of Health, Environmental Health Engineering Department, Birjand University of Medical Sciences, Birjand, Iran.
⁵ Department for Management of Science and Technology Development, Ton Duc Thang University, Ho Chi Minh City, Viet Nam; Faculty of Applied Sciences, Ton Duc Thang University, Ho Chi Minh City, Viet Nam. Electronic address: azam.marjani@tdtu.edu.vn.
⁶ Department of Chemical Sciences, Bernal Institute, University of Limerick, Limerick, Ireland.
⁷ Department of Chemical Sciences, Bernal Institute, University of Limerick, Limerick, Ireland; Laboratory of Computational Modeling of Drugs, South Ural State University, 76 Lenin prospekt, Chelyabinsk 454080, Russia.

PMID: 33461011
DOI: 10.1016/j.jhazmat.2021.125074

Abstract

High-performance novel iron oxyhydroxide (limonite) nanostructure, with improved surface reactive sites, was prepared via one-pot, eco-friendly, free precursor and cold glow discharge N₂-plasma technique. Natural and plasma treated (PTNL/N₂) limonite samples were characterized by FESEM, XPS, XRD, FTIR, AAS, EDX, BET/BJH and pH_pzc to confirm the successful synthesis. Central composite design (CCD) and artificial neural network (ANN, topology of 4:8:1) methods were utilized to study the oxidation/mineralization of phenazopyridine (PhP) as a hazardous contaminant by heterogeneous catalytic ozonation process (HCOP). The obtained results indicated that PTNL/N₂ had the highest catalytic performance in PhP degradation (98.6% in 40 min) and mineralization (80.4% in 120 min). The degradation mechanism in different processes was investigated by dissolved ozone concentration, various organic scavengers (BQ and TBA) and inorganic salts (NaNO₃, NaCl, Na₂CO₃ and NaH₂PO₄). Moreover, reusability-stability, Fe and nitrogen (NO₃^- and NH₄⁺) ions release were assessed during different AOPs. Furthermore, toxicity tests indicated that the HCOP using PTNL/N₂ was able to detoxify the PhP solutions efficiently. Finally, Density Functional Theory (DFT) studies were employed to introduce the most plausible contaminant degradation pathway, reactive sites and byproducts. This research provided a new insight into the improvement of wastewater treatment studies by a combination of experiment and computer simulation.

Keywords: Density functional theory; Heterogeneous catalytic ozonation processes; N(2)-plasma treatment technology; Natural limonite nanostructure; Pharmaceutical pollutant.

Publication types

Research Support, Non-U.S. Gov't