Effective advance treatment of secondary effluent from industrial parks by the Mn-based catalyst ozonation process

doi:10.1007/s11783-024-1884-4

Front. Environ. Sci. Eng.

2024, Vol. 18

Issue (10) : 124 https://doi.org/10.1007/s11783-024-1884-4

Effective advance treatment of secondary effluent from industrial parks by the Mn-based catalyst ozonation process

Zhijuan Niu^1,², Shihao Han¹, Weihua Qin³, Pan Gao⁴, Feng Xiao¹, Shaoxia Yang¹(

)

¹. School of Water Resources and Hydropower Engineering, North China Electric Power University, Beijing 102206, China
². Research Center for Eco-Environmental Engineering, Dongguan University of Technology, Dongguan 523808, China
³. CCCC Highway Consultants Co., Ltd., Beijing 100010, China
⁴. National Engineering Laboratory for Biomass Power Generation Equipment, School of Renewable Energy, North China Electric Power University, Beijing 102206, China

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Abstract

● Catalytic ozonation could effectively purify the secondary effluent from IPWWTPs.

● High removal on COD, UV₂₅₄ and TOC were obtained in the Mn-based catalyst/O₃ system.

● Mn-based catalytic ozonation preferred to degrade aromatic contaminants in wastewater.

● ·O₂^‒/HO₂· and ¹O₂ dominated contaminants removal in the Mn-based catalyst/O₃ system.

Catalytic ozonation is a potential technology to eliminate refractory organic contaminants with the low concentration in secondary effluent from industrial park wastewater treatment plants (IPWWTPs). In this study, the catalytic ozonation over the Mn-based catalyst significantly improved the chemical oxygen demand (COD), total organic carbon (TOC), and UV₂₅₄ removals of secondary effluent from IPWWTPs. The Mn-based catalyst/O₃ system achieved 84.8%, 69.8%, and 86.4% removals of COD, TOC, and UV₂₅₄, which were 3.3, 5.7, and 1.1 times that in ozonation alone, respectively. Moreover, the Mn-based catalytic ozonation process exhibited excellent pH tolerance ranging from pH 4.0 to 9.0. Additionally, the depth analysis based on fluorescence excitation-emission matrix (EEM) confirmed that the catalytic ozonation process preferred to degrade toxic aromatic hydrocarbons. The existence of the Mn-based catalyst/O₃ system enhanced 21.4%–38.3% more fluorescent organic matters removal, compared to that in ozonation alone. Mechanistic studies proved that the abundant Lewis acid sites (Mnⁿ⁺/Mn⁽ⁿ⁺¹⁾⁺ and adsorbed oxygen) on the surface of the Mn-based catalyst effectively promoted O₃ decomposition into reactive oxygen species (ROS), and ·O₂^‒/HO₂· and ¹O₂ were the main ROS for degrading refractory organic contaminants. The contributions of ROS oxidation (91.2%) was much higher than that of direct O₃ oxidation (8.8%). Thus, this work provides an effective advanced treatment process for purifying secondary effluent from IPWWTPs.

Keywords Catalytic ozonation Mn-based catalyst Secondary effluent Industrial park wastewater

Corresponding Author(s): Shaoxia Yang

Issue Date: 18 July 2024

Cite this article:

Zhijuan Niu,Shihao Han,Weihua Qin, et al. Effective advance treatment of secondary effluent from industrial parks by the Mn-based catalyst ozonation process[J]. Front. Environ. Sci. Eng., 2024, 18(10): 124.

URL:

https://academic.hep.com.cn/fese/EN/10.1007/s11783-024-1884-4
https://academic.hep.com.cn/fese/EN/Y2024/V18/I10/124

Fig.1 Impacts of ozone dosage on the COD removal (a) and ozone utilization efficiency (b) in ozonation alone process (pH = 4.0, t = 25 °C); COD removal (c), the kinetics curves for COD removal (d), TOC removal (e) and UV₂₅₄ removal (f) in catalytic ozonation process over different catalysts ([O₃] = 0.84 g/h, [Catalyst] = 100 g/L, pH = 4.0, t = 25 °C).

Fig.2 Impacts of operating conditions on the COD removal in secondary effluent from IPWWTPs in the Mn-based catalytic ozonation process: Catalyst dosage (a) and the kinetics curves for COD removal in different catalyst dosages (b). ([O₃] = 0.84 g/h, pH = 4.0, t = 25 °C); pH value (c) and the kinetics curves for COD removal in different initial pH values (d). ([O₃] = 0.84 g/h, [Catalyst] = 100 g/L, t = 25 °C).

Fig.3 Stability of the Mn-based catalyst in catalytic ozonation of secondary effluent from IPWWTPs. ([O₃] = 0.84 g/h, [Catalyst] = 100 g/L, pH = 4.0, t = 25 °C).

Fig.4 EEM spectra of secondary effluent from IPWWTPs treated by the Mn-based catalytic ozonation process: Influent: raw water (a); the removal of fluorescent substances in different reaction time by ozonation alone process and the catalytic ozonation process (b); Effluent: by ozonation alone process for 20 min (c), 40 min (e), and 60 min (g); Effluent: by the Mn-based catalyst catalytic ozonation process for 20 min (d), 40 min (f), and 60 min (h), respectively. ([O₃] = 0.84 g/h, [Catalyst] = 100 g/L, pH = 4.0, t = 25 °C).

Fig.5 Morphological characterization and high-resolution XPS spectra of the Mn-based catalyst: SEM images of the catalyst (a); EDS images of the catalyst (b); Mn 2p (c) and O 1s (e) XPS spectra of the fresh and used catalysts; the relative content of different chemical state for Mn (d) and O (f) on the fresh and used catalysts.

Fig.6 Identification of dominant active species in the Mn-based catalyst/O₃ process: impacts of PO₄^3─ on the COD degradation (a) ([O₃] = 0.84 g/h, [Catalyst] = 100 g/L, pH = 4.0, t = 25 °C). Impacts of different radical scavengers on the CIP degradation in secondary effluent from IPWWTPs over the Mn-based catalyst/O₃ process (b) ([CIP]₀ = 60 mg/L, [O₃] = 0.84 g/h, [Catalyst] = 100 g/L, pH = 4.0, t = 25 °C). ESR spectra for detection of ROS in the Mn-based catalytic ozonation process (c) ([O₃] = 0.84 g/h, [Catalyst] = 100 g/L, pH = 4.0, t = 25 °C).

Fig.7 Possible mechanism for contaminants removal in the catalytic ozonation process over the Mn-based catalyst.

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