Effective advance treatment of secondary effluent from industrial parks by the Mn-based catalyst ozonation process
Zhijuan Niu, Shihao Han, Weihua Qin, Pan Gao, Feng Xiao, Shaoxia Yang
Effective advance treatment of secondary effluent from industrial parks by the Mn-based catalyst ozonation process
● 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.
Catalytic ozonation / Mn-based catalyst / Secondary effluent / Industrial park wastewater
[1] |
Agarkoti C, Gogate P R, Pandit A B. (2022). Coupling of acoustic/hydrodynamic cavitation with ozone (O3), hydrogen peroxide (H2O2), magnesium oxide (MgO) and manganese dioxide (MnO2) for the effective treatment of CETP effluent. Separation and Purification Technology, 284: 120281
CrossRef
Google scholar
|
[2] |
Chen W, Westerhoff P, Leenheer J A, Booksh K. (2003). Fluorescence excitation-emission matrix regional integration to quantify spectra for dissolved organic matter. Environmental Science & Technology, 37(24): 5701–5710
CrossRef
Google scholar
|
[3] |
Chen X Y, Dong M X, Zhang L, Luan X Y, Cui X W, Cui Z J. (2022). Comprehensive evaluation of environmental and economic benefits of industrial symbiosis in industrial parks. Journal of Cleaner Production, 354: 131635
CrossRef
Google scholar
|
[4] |
Fuentes Barrera G A, Gabarrell i Durany X, Rieradevall Pons J, Guerrero Erazo J G. (2021). Trends in global research on industrial parks: a bibliometric analysis from 1996–2019. Heliyon, 7(8): e07778
CrossRef
Google scholar
|
[5] |
Fu L Y, Wu C Y, Zhou Y X, Zuo J, Song G Q, Tan Y. (2019). Ozonation reactivity characteristics of dissolved organic matter in secondary petrochemical wastewater by single ozone, ozone/H2O2, and ozone/catalyst. Chemosphere, 233: 34–43
CrossRef
Google scholar
|
[6] |
Guan Z J, Guo Y P, Mo Z H, Chen S J, Liang J L, Liao X J, Zhang Y M, Huang Z H, Song W F, Xu Y B.
CrossRef
Google scholar
|
[7] |
Han Y, Yang Y, Liu W B, Hou Y L, Wang C, Shang J W, Cheng X W. (2024). Degradation of Rhodamine B by MnFe-LDH/PMS/O3 three-phase catalytic system: performance, mechanism and ecotoxicity studies. Frontiers of Environmental Science & Engineering, 18(1): 9
CrossRef
Google scholar
|
[8] |
He C, Wang J B, Wang C R, Zhang C H, Hou P, Xu X Y. (2020). Catalytic ozonation of bio-treated coking wastewater in continuous pilot- and full-scale system: efficiency, catalyst deactivation and in-situ regeneration. Water Research, 183: 116090
CrossRef
Google scholar
|
[9] |
He Y N, Chen Y, Li J Z, Wang D, Song S, Dong F L, He Z Q. (2023). Efficient degradation of 2,3,5-trimethylpyrazine by catalytic ozonation over MnOx supported on biochar derived from waste tea leaves. Chemical Engineering Journal, 464: 142525
CrossRef
Google scholar
|
[10] |
Hu W Q, Tian J P, Zang N, Gao Y, Chen L J. (2019). Study of the development and performance of centralized wastewater treatment plants in Chinese industrial parks. Journal of Cleaner Production, 214: 939–951
CrossRef
Google scholar
|
[11] |
Huang Y J, Luo M H, Li S Z, Xia D H, Tang Z Y, Hu S Y, Ye S T, Sun M J, He C, Shu D. (2021). Efficient catalytic activity and bromate minimization over lattice oxygen-rich MnOOH nanorods in catalytic ozonation of bromide-containing organic pollutants: lattice oxygen-directed redox cycle and bromate reduction. Journal of Hazardous Materials, 410: 124545
CrossRef
Google scholar
|
[12] |
Jothinathan L, Cai Q Q, Ong S L, Hu J Y. (2022). Fe-Mn doped powdered activated carbon pellet as ozone catalyst for cost-effective phenolic wastewater treatment: mechanism studies and phenol by-products elimination. Journal of Hazardous Materials, 424: 127483
CrossRef
Google scholar
|
[13] |
Li C H, Jiang F, Sun D Z, Qiu B. (2017). Catalytic ozonation for advanced treatment of incineration leachate using (MnO2-Co3O4)/AC as a catalyst. Chemical Engineering Journal, 325: 624–631
CrossRef
Google scholar
|
[14] |
Li L, Wang Y, Zhang W J, Yu S L, Wang X Y, Gao N Y. (2020). New advances in fluorescence excitation-emission matrix spectroscopy for the characterization of dissolved organic matter in drinking water treatment: a review. Chemical Engineering Journal, 381: 122676
CrossRef
Google scholar
|
[15] |
Liu H B, Wang H N, Zhou X, Fan J L, Liu Y F, Yang Y. (2019a). A comprehensive index for evaluating and enhancing effective wastewater treatment in two industrial parks in China. Journal of Cleaner Production, 230: 854–861
CrossRef
Google scholar
|
[16] |
Liu X L, Guo Z, Zhou L B, Yang J, Cao H B, Xiong M, Xie Y B, Jia G R. (2019b). Hierarchical biomimetic BiVO4 for the treatment of pharmaceutical wastewater in visible-light photocatalytic ozonation. Chemosphere, 222: 38–45
CrossRef
Google scholar
|
[17] |
Liu Y, Shen J M, Chen Z L, Liu Y. (2011). Degradation of p-chloronitrobenzene in drinking water by manganese silicate catalyzed ozonation. Desalination, 279(1−3): 219–224
CrossRef
Google scholar
|
[18] |
Liu Y, Wang C M, Guo R, Li J X, Zhao Q, Wang W Q, Qi F, Liu H F, Li Y, Zheng H F. (2022). Heterogeneous catalysis of ozone using iron–manganese silicate for degradation of acrylic acid. Molecules, 27(15): 4973
CrossRef
Google scholar
|
[19] |
Liu Z Q, Huang C X, Li J Y, Yang J J, Qu B, Yang S Q, Cui Y H, Yan Y H, Sun S Q, Wu X H. (2021). Activated carbon catalytic ozonation of reverse osmosis concentrate after coagulation pretreatment from coal gasification wastewater reclamation for zero liquid discharge. Journal of Cleaner Production, 286: 124951
CrossRef
Google scholar
|
[20] |
Long X J, Luo J, Zhong Z X, Zhu Y X, Zhang C J, Wan J, Zhou H Y, Zhang B P, Xia D S. (2023). Performance and mechanism of carbamazepine removal by FeS-S2O82– process: experimental investigation and DFT calculations. Frontiers of Environmental Science & Engineering, 17(9): 113
CrossRef
Google scholar
|
[21] |
Ly Q V, Nghiem L D, Sibag M, Maqbool T, Hur J. (2018). Effects of COD/N ratio on soluble microbial products in effluent from sequencing batch reactors and subsequent membrane fouling. Water Research, 134: 13–21
CrossRef
Google scholar
|
[22] |
Nawaz F, Cao H B, Xie Y B, Xiao J D, Chen Y, Ghazi Z A. (2017). Selection of active phase of MnO2 for catalytic ozonation of 4-nitrophenol. Chemosphere, 168: 1457–1466
CrossRef
Google scholar
|
[23] |
NDRC (2018). Audit Notice Catalogue of Chinese Development Zones. Beijing: National Development and Reform Commission
|
[24] |
Pang Z J, Luo P, Wei C, Qin Z, Wei T, Hu Y, Wu H Z, Wei C H. (2022). In-situ growth of Co/Ni bimetallic organic frameworks on carbon spheres with catalytic ozonation performance for removal of bio-treated coking wastewater. Chemosphere, 291: 132874
CrossRef
Google scholar
|
[25] |
Panjwani M K, Wang Q, Ma Y M, Lin Y X, Xiao F, Yang S X. (2021). High degradation efficiency of sulfamethazine with the dual-reaction-center Fe-Mn-SiO2 Fenton-like nanocatalyst in a wide pH range. Environmental Science. Nano, 8(8): 2204–2213
CrossRef
Google scholar
|
[26] |
Qiu J K, Wang J, Ren M Z, Yang X, Zhang J B, Zhang X L, Cao H B, Xie Y B. (2023). Comprehensive effect of water matrix on catalytic ozonation of chloride contained saline wastewater. Water Research, 234: 119827
CrossRef
Google scholar
|
[27] |
Ren T F, Ouyang C P, Zhou Z Y, Chen S N, Yin M X, Huang X, Zhang X Y. (2023). Mn-doped carbon-Al2SiO5 fibers enable catalytic ozonation for wastewater treatment: Interface modulation and mass transfer enhancement. Journal of Hazardous Materials, 460: 132307
CrossRef
Google scholar
|
[28] |
Shen T D, Su W T, Yang Q Q, Ni J, Tong S P. (2020). Synergetic mechanism for basic and acid sites of MgMxOy (M=Fe, Mn) double oxides in catalytic ozonation of p-hydroxybenzoic acid and acetic acid. Applied Catalysis B: Environmental, 279: 119346
CrossRef
Google scholar
|
[29] |
Su P, Fu W Y, Hu Z Z, Jing J A, Zhou M H. (2022). Insights into transition metal encapsulated N-doped CNTs cathode for self-sufficient electrocatalytic degradation. Applied Catalysis B: Environmental, 313: 121457
CrossRef
Google scholar
|
[30] |
Su T, Wang Z K, Zhou K, Chen X N, Cheng Y, Zhang G C, Wu D W, Sun S P. (2021). Advanced treatment of secondary effluent organic matters (EfOM) from an industrial park wastewater treatment plant by Fenton oxidation combining with biological aerated filter. Science of the Total Environment, 784: 147204
CrossRef
Google scholar
|
[31] |
Sun Z Q, Zhao L, Liu C H, Zhen Y F, Ma J. (2019). Catalytic ozonation of ketoprofen with in situ N-doped carbon: a novel synergetic mechanism of hydroxyl radical oxidation and an intra-electron-transfer nonradical reaction. Environmental Science & Technology, 53(17): 10342–10351
CrossRef
Google scholar
|
[32] |
Tian S Q, Qi J Y, Wang Y P, Liu Y L, Wang L, Ma J. (2021). Heterogeneous catalytic ozonation of atrazine with Mn-loaded and Fe-loaded biochar. Water Research, 193: 116860
CrossRef
Google scholar
|
[33] |
Wang D, Yang Z, He Y N, Dong S W, Dong F L, He Z Q, Lu X H, Wang L Z, Song S, Ma J. (2023). Metribuzin and metamitron degradation using catalytic ozonation over tourmaline: kinetics, degradation pathway, and toxicity. Separation and Purification Technology, 309: 123028
CrossRef
Google scholar
|
[34] |
Wang J L, Chen H. (2020). Catalytic ozonation for water and wastewater treatment: recent advances and perspective. Science of the Total Environment, 704: 135249
CrossRef
Google scholar
|
[35] |
Wang Y C, Wang Y K, Lu X, Sun W Q, Xu Y H, Zhou J, Sun Y J. (2022). Catalytic ozonation for effective degradation of coal chemical biochemical tail water by Mn/Ce@RM catalyst. Water, 14(2): 206
CrossRef
Google scholar
|
[36] |
Xie J X, Chen W R, Lv Y F, Chen H Y, Li X K, Li L S. (2021). Synthesis of CeOx@SiO2 with tandem effect of mass transfer and activation for enhancing sulfanilamide degradation with ozone. Separation and Purification Technology, 256: 117823
CrossRef
Google scholar
|
[37] |
Yan Z C, Zhu J X, Hua X Y, Liang D P, Dong D M, Guo Z Y, Zheng N, Zhang L W. (2020). Catalytic ozonation for the degradation of polyvinyl alcohol in aqueous solution using catalyst based on copper and manganese. Journal of Cleaner Production, 272: 122856
CrossRef
Google scholar
|
[38] |
Yang J, Xiao J D, Cao H B, Guo Z, Rabeah J, Bruckner A, Xie Y B. (2018). The role of ozone and influence of band structure in WO3 photocatalysis and ozone integrated process for pharmaceutical wastewater treatment. Journal of Hazardous Materials, 360: 481–489
CrossRef
Google scholar
|
[39] |
Yang S, Nie J Q, Wei F, Yang X D. (2016). Removal of ozone by carbon nanotubes/quartz fiber film. Environmental Science & Technology, 50(17): 9592–9598
CrossRef
Google scholar
|
[40] |
Yao J, Zhang Y, Dong Z K. (2021). Enhanced degradation of contaminants of emerging concern by electrochemically activated peroxymonosulfate: performance, mechanism, and influencing factors. Chemical Engineering Journal, 415: 128938
CrossRef
Google scholar
|
[41] |
Yuan Y C, Liu J D, Gao B, Sillanpää M. (2022). Landfill leachate treatment in-depth by bio-chemical strategy: microbial activation and catalytic ozonation mechanism. Chemical Engineering Journal, 444: 136464
CrossRef
Google scholar
|
[42] |
Zhang D P, Liu Y D, Song Y Y, Sun X B, Liu W, Duan J, Cai Z Q. (2023a). Synergistic effect of Fe and Ce on Fe doped CeO2 for catalytic ozonation of amoxicillin: efficiency evaluation and mechanism study. Separation and Purification Technology, 313: 123430
CrossRef
Google scholar
|
[43] |
Zhang J, Liu M Q, Pang B, Liu C, Ma J J, Niu J R, Zhang R A. (2023b). Ciprofloxacin degradation in microbubble ozonation combined with electro-generated H2O2 process: operational parameters and oxidation mechanism. Separation and Purification Technology, 325: 124676
CrossRef
Google scholar
|
[44] |
Zhang J L, Xiong Z K, Wei J, Song Y H, Ren Y Z, Xu D Y, Lai B. (2020). Catalytic ozonation of penicillin G using cerium-loaded natural zeolite (CZ): efficacy, mechanisms, pathways and toxicity assessment. Chemical Engineering Journal, 383: 123144
CrossRef
Google scholar
|
[45] |
Zhao K H, Ma Y L, Lin F, Ge S Y, Zhu L. (2021). Refractory organic compounds in coal chemical wastewater treatment by catalytic ozonation using Mn-Cu-Ce/Al2O3. Environmental Science and Pollution Research International, 28(30): 41504–41515
CrossRef
Google scholar
|
[46] |
Zhou K, Wang Z K, Wang X N, Jiao G L, Li Y F, Sun S P, Chen X D. (2020). Degradation of emerging pharmaceutical micropollutants in municipal secondary effluents by low-pressure UVC-activated HSO5− and S2O82− AOPs. Chemical Engineering Journal, 393: 124712
CrossRef
Google scholar
|
[47] |
Zhou Y F, Qin W H, Sun X L, Zhu Y Q, Niu J F. (2022). Synergistic effects on d-band center via coordination sites of M-N3P1 (M = Co and Ni) in dual single atoms that enhances photocatalytic dechlorination from tetrachlorobispheonl A. Journal of Hazardous Materials, 430: 128419
CrossRef
Google scholar
|
[48] |
Zhou Z Y, Yan N, Yin M X, Ren T F, Chen S N, Lu K C, Cao X X, Huang X, Zhang X Y. (2023). Catalytic ozonation in advanced treatment of kitchen wastewater: multi-scale simulation and pilot-scale study. Frontiers of Environmental Science & Engineering, 17(12): 146
CrossRef
Google scholar
|
[49] |
Zhu G X, Zhu W, Lou Y, Ma J, Yao W Q, Zong R L, Zhu Y F. (2021). Encapsulate α-MnO2 nanofifiber within graphene layer to tune surface electronic structure for efficient ozone decomposition. Nature Communications, 12(1): 4152
CrossRef
Google scholar
|
/
〈 | 〉 |