Electro-catalytic activity of CeO_x modified graphite felt for carbamazepine degradation via E-peroxone process

Highlights

•CeO_x/GF-EP process had the better degradation efficiency than GF-EP process.

•CeO_x/GF-EP process had the flexible application in the pH range from 5.0 to 9.0.

•CeO_x could enhance surface hydrophilicity and reduce the charge-transfer resistance.

•The interfacial electron transfer process was revealed.

Abstract

E-peroxone (EP) was one of the most attractive AOPs for removing refractory organic compounds from water, but the high energy consumption for in situ generating H₂O₂ and its low reaction efficiency for activating O₃ under acidic conditions made the obstacles for its practical application. In this study, cerium oxide was loaded on the surface of graphite felt (GF) by the hydrothermal method to construct the efficient electrode (CeO_x/GF) for mineralizing carbamazepine (CBZ) via EP process. CeO_x/GF was an efficient cathode, which led to 69.4% TOC removal in CeO_x/GF-EP process with current intensity of 10 mA in 60 min. Moreover, CeO_x/GF had the flexible application in the pH range from 5.0 to 9.0, TOC removal had no obvious decline with decrease of pH. Comparative characterizations showed that CeO_x could enhance surface hydrophilicity and reduce the charge-transfer resistance of GF. About 5.4 mg/L H₂O₂ generated in CeO_x/GF-EP process, which was 2.1 times as that in GF-EP process. The greater ozone utility was also found in CeO_x/GF-EP process. More O₃ was activated into hydroxyl radicals, which accounted for the mineralization of CBZ. An interfacial electron transfer process was revealed, which involved the function of oxygen vacancies and Ce³⁺/Ce⁴⁺ redox cycle. CeO_x/GF had the good recycling property in fifth times’ use.

Graphical abstract

Keywords

E-peroxone / CeO_x / Graphite felt / Carbamazepine / Mineralization

References

[1] Afzal S, Quan X, Lu S (2019). Catalytic performance and an insight into the mechanism of CeO₂ nanocrystals with different exposed facets in catalytic ozonation of p-nitrophenol. Applied Catalysis B: Environmental, 248: 526–537

[2] Bader H, Hoigné J (1981). Determination of ozone in water by the indigo method. Water Research, 15(4): 449–456

[3] Bourgin M, Borowska E, Helbing J, Hollender J, Kaiser H P, Kienle C, Mcardell C S, Simon E, Von Gunten U (2017). Effect of operational and water quality parameters on conventional ozonation and the advanced oxidation process O₃/H₂O₂: Kinetics of micropollutant abatement, transformation product and bromate formation in a surface water. Water Research, 122: 234–245

[4] Brillas E, Casado J (2002). Aniline degradation by Electro-Fenton and peroxi-coagulation processes using a flow reactor for wastewater treatment. Chemosphere, 47(3): 241–248

[5] Chen N, Zhang H, Luo X D, Sun C Y (2020). SiO₂-decorated graphite felt electrode by silicic acid etching for iron-chromium redox flow battery. Electrochimica Acta, 336: 135646

[6] Ding X, Gutierrez L, Croue J P, Li M, Wang L, Wang Y (2020). Hydroxyl and sulfate radical-based oxidation of RhB dye in UV/H₂O₂ and UV/persulfate systems: Kinetics, mechanisms, and comparison. Chemosphere, 253: 126655

[7] Ding Y, Wang J, Xu S, Lin K Y A, Tong S (2018). Oxygen vacancy of CeO₂ improved efficiency of H₂O₂/O₃ for the degradation of acetic acid in acidic solutions. Separation and Purification Technology, 207: 92–98

[8] Fan X, Gao J, Li W, Huang J, Yu G (2020). Determination of 27 pharmaceuticals and personal care products (PPCPs) in water: The benefit of isotope dilution. Frontiers of Environmental Science & Engineering, 14(1): 8

[9] Feng H, Liu M, Zeng W, Chen Y (2021). Optimization of the O3/H2O2 process with response surface methodology for pretreatment of mother liquor of gas field wastewater. Frontiers of Environmental Science & Engineering, 15(4): 78 doi.org/10.1007/s11783-020-1371-5

[10] Gao C, Wang N, Peng S, Liu S, Lei Y, Liang X, Zeng S, Zi H (2013). Influence of Fenton’s reagent treatment on electrochemical properties of graphite felt for all vanadium redox flow battery. Electrochimica Acta, 88: 193–202

[11] Ghalebizade M, Ayati B (2019). Acid Orange 7 treatment and fate by electro-peroxone process using novel electrode arrangement. Chemosphere, 235: 1007–1014

[12] Guo Z, Zhou L, Cao H, Xie Y, Xiao J, Yang J, Zhang Y (2018). C₃N₄–Mn/CNT composite as a heterogeneous catalyst in the electro-peroxone process for promoting the reaction between O₃ and H₂O₂ in acid solution. Catalysis Science & Technology, 8(23): 6241–6251

[13] Jiang X, Qu Y, Liu L, He Y, Li W, Huang J, Yang H, Yu G (2019). PPCPs in a drinking water treatment plant in the Yangtze River Delta of China: Occurrence, removal and risk assessment. Frontiers of Environmental Science & Engineering, 13(2): 27 doi.org/10.1007/s11783-019-1109-4

[14] Li D, Zheng T, Liu Y, Hou D, Yao K K, Zhang W, Song H, He H, Shi W, Wang L, Ma J (2020a). A novel Electro-Fenton process characterized by aeration from inside a graphite felt electrode with enhanced electrogeneration of H₂O₂ and cycle of Fe³⁺/Fe²⁺. Journal of Hazardous Materials, 396: 122591

[15] Li S, Huang J, Li X, Li L (2020b). The relation of interface electron transfer and PMS activation by the H-bonding interaction between composite metal and MCM-48 during sulfamethazine ozonation. Chemical Engineering Journal, 398: 125529

[16] Li Y, Wu L, Wang Y, Ke P, Xu J, Guan B (2020c). g-Al₂O₃ doped with cerium to enhance electron transfer in catalytic ozonation of phenol. Journal of Water Process Engineering, 36: 101313

[17] Liang X, Wang P, Gao Y, Huang H, Tong F, Zhang Q, Wang Z, Liu Y, Zheng Z, Dai Y, Huang B (2020). Design and synthesis of porous M-ZnO/CeO₂ microspheres as efficient plasmonic photocatalysts for nonpolar gaseous molecules oxidation: Insight into the role of oxygen vacancy defects and M=Ag, Au nanoparticles. Applied Catalysis B: Environmental, 260: 118151

[18] Liu X, Xie L, Liu Y, Zhao P, Han Y, Cheng S, Bai X, Li Y (2020). Rapid preparation of highly stable ZnO-CeO₂/CF cathode by one-step electro-deposition for efficient degradation of ciprofloxacin in electro-Fenton system. Catalysis Today, 355: 458–465

[19] Liu Z, Zhao C, Wang P, Zheng H, Sun Y, Dionysiou D D (2018). Removal of carbamazepine in water by electro-activated carbon fiber-peroxydisulfate: Comparison, optimization, recycle, and mechanism study. Chemical Engineering Journal, 343: 28–36

[20] Mi X, Han J, Sun Y, Li Y, Hu W, Zhan S (2019). Enhanced catalytic degradation by using RGO-Ce/WO₃ nanosheets modified CF as electro-Fenton cathode: Influence factors, reaction mechanism and pathways. Journal of Hazardous Materials, 367: 365–374

[21] Pan F, Ji H, Du P, Huang T, Wang C, Liu W (2021). Insights into catalytic activation of peroxymonosulfate for carbamazepine degradation by MnO₂ nanoparticles in-situ anchored titanate nanotubes: Mechanism, ecotoxicity and DFT study. Journal of Hazardous Materials, 402: 123779

[22] Peng R, Shen T, Tong S, Ma C (2016). An effective heterogeneous ozone-based advanced oxidation process in acidic solution—Ti-MCM-41/H₂O₂/O₃. Ozone Science and Engineering, 38(3): 194–202

[23] Savchenko D, Vorlíček V, Prokhorov A, Kalabukhova E, Lančok J, Jelínek M (2018). Raman and EPR spectroscopic studies of chromium-doped diamond-like carbon films. Diamond and Related Materials, 83: 30–37

[24] Song Y, Gong H, Wang J, Chang F, Wang K (2020). Enhanced triallyl isocyanurate (TAIC) degradation through application of an O3/UV process: Performance optimization and degradation pathways. Frontiers of Environmental Science & Engineering, 14(4): 64 doi.org/10.1007/s11783-020-1243-z

[25] Sun S, Yao H, Fu W, Liu F, Wang X, Zhang W (2020). Enhanced degradation of carbamazepine in FeOCl based Photo-Fenton reaction. Journal of Environmental Chemical Engineering, 9: 104501

[26] Tan Z, Zhang J, Chen Y C, Chou J P, Peng Y K (2020). Unravelling the role of structural geometry and chemical state of well-defined oxygen vacancies on pristine CeO₂ for H₂O₂ activation. Journal of Physical Chemistry Letters, 11(14): 5390–5396

[27] Trojanowicz M (2020). Removal of persistent organic pollutants (POPs) from waters and wastewaters by the use of ionizing radiation. Science of the Total Environment, 718: 134425

[28] Wang J, Chen H (2020). Catalytic ozonation for water and wastewater treatment: Recent advances and perspective. Science of the Total Environment, 704: 135249

[29] Wang Y, Yu G, Deng S, Huang J, Wang B (2018). The electro-peroxone process for the abatement of emerging contaminants: Mechanisms, recent advances, and prospects. Chemosphere, 208: 640–654

[30] Wang Y, Zhou W, Gao J, Ding Y, Kou K (2019). Oxidative modification of graphite felts for efficient H₂O₂ electrogeneration: Enhancement mechanism and long-term stability. Journal of Electroanalytical Chemistry (Lausanne, Switzerland), 833: 258–268

[31] Xia G, Wang H, Zhan J, Yin X, Wu X, Yu G, Wang Y, Wu M (2020). Evaluation of the stability of polyacrylonitrile-based carbon fiber electrode for hydrogen peroxide production and phenol mineralization during electro-peroxone process. Chemical Engineering Journal, 396: 125291

[32] Xie J, Li X, Chen W, Sun X, Chen K, Tang Y, Li L (2020). Enhanced mineralization of oxalate by heterogeneous peroxone: The interfacial reaction on the core-shell CeO_x@SiO₂. Chemical Engineering Journal, 379: 122344

[33] Yue L, Li W, Sun F, Zhao L, Xing L (2010). Highly hydroxylated carbon fibres as electrode materials of all-vanadium redox flow battery. Carbon, 48(11): 3079–3090

[34] Zeng Q, Wang X, Jin M, Akinoglu E M, Zhou G, Shui L (2020). Nitrogen defects-rich porous graphitic carbon nitride for efficient photocatalytic hydrogen evolution. Journal of Colloid and Interface Science, 578: 788–795

[35] Zhang Z, Chen H, Wang J, Zhang Y (2020). Degradation of carbamazepine by combined radiation and persulfate oxidation process. Radiation Physics and Chemistry, 170: 108639

[36] Zhou J, An X, Lan H, Liu H, Qu J (2020). New insights into the surface-dependent activity of graphitic felts for the electro-generation of H₂O₂. Applied Surface Science, 509: 144875

[37] Zhou L, Zhou M, Hu Z, Bi Z, Serrano K G (2014). Chemically modified graphite felt as an efficient cathode in electro-Fenton for p-nitrophenol degradation. Electrochimica Acta, 140: 376–383

[38] Zhou Q, Wang Q, Tong S (2017). Mn²⁺/H₂O₂/O₃, a high efficient advanced oxidation process in acidic solution. Journal of Environmental Chemical Engineering, 5(1): 924–930

[39] Zou X, Li X, Chen C, Zhu X, Huang X, Wu Y, Pi Z, Chen Z, Tao Z, Wang D, Yang Q (2020). Degradation performance of carbamazepine by ferrous-activated sodium hypochlorite: Mechanism and impacts on the soil system. Chemical Engineering Journal, 389: 123451

Acknowledgements

This study was funded by the National Natural Science Foundation (No. 51978288), Natural Science Foundation of Guangdong Province (No. 2019A1515012202), Major Science and Technology Program for Water Pollution Control and Treatment in China (No. 2017ZX07202-004).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11783-021-1410-x and is accessible for authorized users.

RIGHTS & PERMISSIONS

2021 Higher Education Press