Catalytic activity of H2O2 by goethite and lepidocrocite: Insight from 5-bromosalicylic acid removal mechanism and density functional theory calculation (ID:CHEM114760)

Wanyi Huang; Yixing Yuan; Dan Zhong; Peng Zhang; Arvin Liangdy; Teik-Thye Lim; Wencheng Ma; Yuan Yuan

doi:10.1016/j.chemosphere.2023.138551

Catalytic activity of H₂O₂ by goethite and lepidocrocite: Insight from 5-bromosalicylic acid removal mechanism and density functional theory calculation (ID:CHEM114760)

Chemosphere. 2023 Jul:329:138551. doi: 10.1016/j.chemosphere.2023.138551. Epub 2023 Mar 30.

Authors

Wanyi Huang¹, Yixing Yuan², Dan Zhong³, Peng Zhang⁴, Arvin Liangdy⁵, Teik-Thye Lim⁶, Wencheng Ma⁷, Yuan Yuan⁸

Affiliations

¹ State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, China. Electronic address: wanyihuang2021@163.com.
² State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, China. Electronic address: yyx1957@163.com.
³ State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, China. Electronic address: zhongdan2001@163.com.
⁴ State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, China. Electronic address: pengzhang329@163.com.
⁵ School of Civil and Environmental Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore, 639798, Singapore; Nanyang Environment and Water Research Institute (NEWRI), Nanyang Technological University, 1 Cleantech Loop, CleanTech One, Singapore, 637141, Singapore. Electronic address: ARVINLIA001@e.ntu.edu.sg.
⁶ School of Civil and Environmental Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore, 639798, Singapore; Nanyang Environment and Water Research Institute (NEWRI), Nanyang Technological University, 1 Cleantech Loop, CleanTech One, Singapore, 637141, Singapore. Electronic address: CTTLim@ntu.edu.sg.
⁷ State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, China. Electronic address: damahit@163.com.
⁸ School of Biological Engineering, Beijing Polytechnic, Beijing, 100176, China. Electronic address: yy1225l@126.com.

PMID: 37003437
DOI: 10.1016/j.chemosphere.2023.138551

Abstract

We have compared the elimination of 5-bromosalicylic acid (BSA) in the systems of goethite (α-FeOOH)/H₂O₂ and lepidocrocite (γ-FeOOH)/H₂O₂. The results demonstrated that BSA (10 mg L^-1) could be successfully adsorbed on α- and γ-FeOOH (0.5 g L^-1) and then effectively degraded after the addition of H₂O₂ (14.7 mM). BSA adsorption on both α- and γ-FeOOH followed pseudo-second order adsorption kinetic models, with γ-FeOOH having greater adsorption ability than α-FeOOH. In the α-FeOOH/H₂O₂ system, BSA degradation was well fitted with the pseudo-second order kinetics, whereas the oxidation in γ-FeOOH/H₂O₂ system had a two-stage pseudo-first order kinetics. Electron paramagnetic resonance (EPR) results for these two systems revealed the presence of •OH and •OOH, and further tests with radical captures demonstrated their dominance in degrading BSA. Based on the electronic structure analysis, electrons were more easily transferred from the H₂O₂ molecule to the Fe atoms of α-FeOOH, explaining the density functional theory (DFT) calculation results, which showed that α-FeOOH performed better in catalyzing the decomposition of H₂O₂. However, the free radicals are more likely to desorb from γ-FeOOH, which made the γ-FeOOH/H₂O₂ system more efficient in degrading BSA.

Keywords: Activation of H(2)O(2); Adsorption; Density functional theory; Heterogenous fenton-like.

MeSH terms

Density Functional Theory
Hydrogen Peroxide* / chemistry
Iron Compounds* / chemistry

Substances

goethite
ferric oxide
Hydrogen Peroxide
Iron Compounds