A heterogeneous double chamber electro-Fenton with high production of H2O2 using La–CeO2 modified graphite felt as cathode

doi:10.1016/j.cjche.2022.04.006

Abstract

Abstract: Hydrogen peroxide synthesis by electro-reduction of O₂ to substitute the current anthraquinone process has attracted a great deal of attention. Low oxygen utilization rate and low hydrogen peroxide production remain obstacles to electro-Fenton application. In situ H₂O₂ generated by electrochemical reaction depends on the electrochemical performance of the cathode and the structure of the reactor. Here, novel graphite felt (GF) modified by La-doped CeO₂ (La–CeO₂) was developed as a cathode. A new double chamber electro-Fenton reactor was proposed, where an organic ultrafiltration membrane was used to prevent H₂O₂ from spreading to the anode. The effects of hydrothermal temperature, time and urea concentration on the electrochemical properties of graphite felt were investigated. The accumulated concentration of H₂O₂ on the modified cathode reached 218.4 mg·L^–1 in 1 h when the optimal conditions of hydrothermal temperature 120 ℃ and urea concentration 0.55% (mass) in 24 h. The degradation rate of methyl orange reached 98.29%. The new electro-Fenton reactor can efficiently produce hydrogen peroxide to degrade various organic substances and has a high potential for treating wastewater in the chemical industry.

Key words: Hydrogen peroxide, Graphite felt modification, Double chamber reactor, Organic ultrafiltration membrane

摘要： Hydrogen peroxide synthesis by electro-reduction of O₂ to substitute the current anthraquinone process has attracted a great deal of attention. Low oxygen utilization rate and low hydrogen peroxide production remain obstacles to electro-Fenton application. In situ H₂O₂ generated by electrochemical reaction depends on the electrochemical performance of the cathode and the structure of the reactor. Here, novel graphite felt (GF) modified by La-doped CeO₂ (La–CeO₂) was developed as a cathode. A new double chamber electro-Fenton reactor was proposed, where an organic ultrafiltration membrane was used to prevent H₂O₂ from spreading to the anode. The effects of hydrothermal temperature, time and urea concentration on the electrochemical properties of graphite felt were investigated. The accumulated concentration of H₂O₂ on the modified cathode reached 218.4 mg·L^–1 in 1 h when the optimal conditions of hydrothermal temperature 120 ℃ and urea concentration 0.55% (mass) in 24 h. The degradation rate of methyl orange reached 98.29%. The new electro-Fenton reactor can efficiently produce hydrogen peroxide to degrade various organic substances and has a high potential for treating wastewater in the chemical industry.

关键词: Hydrogen peroxide, Graphite felt modification, Double chamber reactor, Organic ultrafiltration membrane

Suhang Jiang, Lijuan Tan, Yujia Tong, Lijian Shi, Weixing Li. A heterogeneous double chamber electro-Fenton with high production of H₂O₂ using La–CeO₂ modified graphite felt as cathode[J]. Chinese Journal of Chemical Engineering, 2023, 54(2): 98-105.

References

[1] J.T. Mefford, A.R. Akbashev, M. Kang, C.L. Bentley, W.E. Gent, H.D. Deng, D.H. Alsem, Y.S. Yu, N.J. Salmon, D.A. Shapiro, P.R. Unwin, W.C. Chueh, Correlative operando microscopy of oxygen evolution electrocatalysts, Nature. 593 (7857) (2021) 67–73.
[2] F.K. Yu, Y. Wang, H.R. Ma, M.H. Zhou, Hydrothermal synthesis of FeS₂ as a highly efficient heterogeneous electro-Fenton catalyst to degrade diclofenac via molecular oxygen effects for Fe(II)/Fe(III) cycle, Sep. Purif. Technol. 248 (2020) 117022.
[3] B. Ou, J.X. Wang, Y. Wu, S. Zhao, Z. Wang, A highly efficient cathode based on modified graphite felt for aniline degradation by electro-Fenton, Chemosphere 235 (2019) 49–57.
[4] F.K. Yu, Y. Chen, Y.W. Pan, Y. Yang, H.R. Ma, A cost-effective production of hydrogen peroxide via improved mass transfer of oxygen for electro-Fenton process using the vertical flow reactor, Sep. Purif. Technol. 241 (2020) 116695.
[5] A. Babuponnusami, K. Muthukumar, Advanced oxidation of phenol: A comparison between Fenton, electro-Fenton, sono-electro-Fenton and photo-electro-Fenton processes, Chem. Eng. J. 183 (2012) 1–9.
[6] E. Brillas, I. Sirés, M.A. Oturan, Electro-Fenton process and related electrochemical technologies based on Fenton's reaction chemistry, Chem. Rev. 109 (12) (2009) 6570–6631.
[7] S.B. Hammouda, C. Salazar, F.P. Zhao, D.L. Ramasamy, E. Laklova, S. Iftekhar, I. Babu, M. Sillanpää, Efficient heterogeneous electro-Fenton incineration of a contaminant of emergent concern-cotinine- in aqueous medium using the magnetic double perovskite oxide Sr₂FeCuO₆ as a highly stable catalayst: Degradation kinetics and oxidation products, Appl. Catal. B Environ. 240 (2019) 201–214.
[8] E.H. Umukoro, M.G. Peleyeju, J.C. Ngila, O.A. Arotiba, Towards wastewater treatment: Photo-assisted electrochemical degradation of 2-nitrophenol and orange II dye at a tungsten trioxide-exfoliated graphite composite electrode, Chem. Eng. J. 317 (2017) 290–301.
[9] S.Q. Han, S.U. Hassan, Y.H. Zhu, S. Zhang, H.G. Liu, S. Zhang, J.F. Li, Z.Y. Wang, C. Zhao, Significance of activated carbon fiber as cathode in electro/Fe³⁺/peroxydisulfate oxidation process for removing carbamazepine in aqueous environment, Ind. Eng. Chem. Res. 58 (42) (2019) 19709–19718.
[10] G.Q. Zhang, F.L. Yang, M.M. Gao, X.H. Fang, L.F. Liu, Electro-Fenton degradation of azo dye using polypyrrole/anthraquinone disulphonate composite film modified graphite cathode in acidic aqueous solutions, Electrochimica Acta. 53 (16) (2008) 5155–5161.
[11] Q. Zhang, M. Zhou, G. Ren, Y. Li, Y. Li, X. Du, Highly efficient electrosynthesis of hydrogen peroxide on a superhydrophobic three-phase interface by natural air diffusion, Nat. Commun. 11 (2020) 1731.
[12] L.L. Cui, P.P. Ding, M. Zhou, W.H. Jing, Energy efficiency improvement on in situ generating H₂O₂ in a double-compartment ceramic membrane flow reactor using cerium oxide modified graphite felt cathode, Chem. Eng. J. 330 (2017) 1316–1325.
[13] X.C. Liu, W.Q. Li, Y.R. Wang, G.N. Zhou, Y.X. Wang, C.S. He, G.M. Wang, Y. Mu, Cathode-introduced atomic H* for Fe(II)-complex regeneration to effective electro-Fenton process at a natural pH, Environ. Sci. Technol. 53 (12) (2019) 6927–6936.
[14] W. Zhou, L. Rajic, X.X. Meng, R. Nazari, Y.W. Zhao, Y. Wang, J.H. Gao, Y.K. Qin, A.N. Alshawabkeh, Efficient H₂O₂ electrogeneration at graphite felt modified via electrode polarity reversal: Utilization for organic pollutants degradation, Chem. Eng. J. 364 (2019) 428–439.
[15] Q.Y. Chen, L. Liu, L.F. Liu, Y.Z. Zhang, A novel UV-assisted PEC-MFC system with CeO₂/TiO₂/ACF catalytic cathode for gas phase VOCs treatment, Chemosphere. 255 (2020) 126930.
[16] N.A. Sazelee, N.H. Idris, M.F. Md Din, M. S Yahya, N.A. Ali, M. Ismail, LaFeO₃ synthesised by solid-state method for enhanced sorption properties of MgH₂, Results Phys. 16 (2020) 102844.
[17] Z.G. Gao, Z.R. Jia, K.K. Wang, X.H. Liu, L. Bi, G.L. Wu, Simultaneous enhancement of recoverable energy density and efficiency of lead-free relaxor-ferroelectric BNT-based ceramics, Chem. Eng. J. 402 (2020) 125951.
[18] X.F. Zhang, M.S. Chen, Q. Zhang, J.Q. Liu, Y.C. Wu, New insights into synergistic effects of La₂O₃ and nitrogen doped carbon for improved redox kinetics in lithium-sulfur batteries: A computational study, Appl. Surf. Sci. 563 (2021) 150172.
[19] D. Selvaraj, A. Somanathan, R. Jeyakumar, G. Kumar, Generation of electricity by the degradation of electro-Fenton pretreated latex wastewater using double chamber microbial fuel cell, Int. J. Energy Res. 44 (15) (2020) 12496–12505.
[20] N. Jaafarzadeh, F. Ghanbari, M. Ahmadi, M. Omidinasab, Efficient integrated processes for pulp and paper wastewater treatment and phytotoxicity reduction: Permanganate, electro-Fenton and Co₃O₄/UV/peroxymonosulfate, Chem. Eng. J. 308 (2017) 142–150.
[21] E. Petrucci, A. da Pozzo, L. di Palma, On the ability to electrogenerate hydrogen peroxide and to regenerate ferrous ions of three selected carbon-based cathodes for electro-Fenton processes, Chem. Eng. J. 283 (2016) 750–758.
[22] L.B. Xie, X.Y. Mi, Y.G. Liu, Y. Li, Y. Sun, S.H. Zhan, W.P. Hu, Highly efficient degradation of polyacrylamide by an Fe-doped Ce_0.75Zr_0.25O₂ solid solution/CF composite cathode in a heterogeneous electro-Fenton process, ACS Appl. Mater. Interfaces. 11 (34) (2019) 30703–30712.
[23] J.Q. Xue, S.W. Ma, Q. Bi, X. Zhang, W.Z. Guan, Y. Gao, Revealing the modification mechanism of La-doped Ti/SnO₂ electrodes related to the microelectronic structure by first-principles calculations, J. Alloys Compd. 747 (2018) 423–430.
[24] A.E. Nogueira, A.R.F. Lima, E. Longo, E.R. Leite, E.R. Camargo, Effect of lanthanum and lead doping on the microstructure and visible light photocatalysis of bismuth titanate prepared by the oxidant peroxide method (OPM), J. Photochem. Photobiol. A Chem. 312 (2015) 55–63.
[25] J.F. Pérez, J. Llanos, C. Sáez, C. López, P. Cañizares, M.A. Rodrigo, The jet aerator as oxygen supplier for the electrochemical generation of H₂O₂, Electrochimica Acta. 246 (2017) 466–474.
[26] S.Y. Kim, H.A. Garcia, C.M. Lopez-Vazquez, C. Milligan, A. Herrera, M. Matosic, J. Curko, D. Brdjanovic, Oxygen transfer performance of a supersaturated oxygen aeration system (SDOX) evaluated at high biomass concentrations, Process. Saf. Environ. Prot. 139 (2020) 171–181.
[27] Y.Y. Chu, D.M. Zhang, L. Liu, Y. Qian, L.L. Li, Electrochemical degradation of m-cresol using porous carbon-nanotube-containing cathode and Ti/SnO₂-Sb₂O₅-IrO₂ anode: Kinetics, byproducts and biodegradability, J. Hazard. Mater. 252-253 (2013) 306–312.
[28] L. Zhou, M.H. Zhou, C. Zhang, Y.H. Jiang, Z.H. Bi, J. Yang, Electro-Fenton degradation of p-nitrophenol using the anodized graphite felts, Chem. Eng. J. 233 (2013) 185–192.
[29] Y. Wang, Y.H. Liu, T.F. Liu, S.Q. Song, X.C. Gui, H. Liu, P. Tsiakaras, Dimethyl phthalate degradation at novel and efficient electro-Fenton cathode, Appl. Catal. B Environ. 156-157 (2014) 1–7.
[30] L. Ma, M.H. Zhou, G.B. Ren, W.L. Yang, L. Liang, A highly energy-efficient flow-through electro-Fenton process for organic pollutants degradation, Electrochimica Acta. 200 (2016) 222–230.
[31] L. Zhou, Z.X. Hu, C. Zhang, Z.H. Bi, T. Jin, M.H. Zhou, Electrogeneration of hydrogen peroxide for electro-Fenton system by oxygen reduction using chemically modified graphite felt cathode, Sep. Purif. Technol. 111 (2013) 131–136.

A heterogeneous double chamber electro-Fenton with high production of H₂O₂ using La–CeO₂ modified graphite felt as cathode

A heterogeneous double chamber electro-Fenton with high production of H₂O₂ using La–CeO₂ modified graphite felt as cathode

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Xiaolin Guo, Zhaoyang Zhang, Pengfei Xing, Shuai Wang, Yibing Guo, Yanxin Zhuang. Kinetic mechanism of copper extraction from methylchlorosilane slurry residue using hydrogen peroxide as oxidant [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 228-234.
[2]	Wei Zhou, Xiaoxiao Meng, Liang Xie, Junfeng Li, Yani Ding, Yanlin Su, Jihui Gao, Guangbo Zhao. Simultaneous utilization of electro-generated O₂ and H₂ for H₂O₂ production: An upgrade of the Pd-catalytic electro-Fenton process for pollutants degradation [J]. Chinese Journal of Chemical Engineering, 2022, 44(4): 363-368.
[3]	Yanqiang Shi, Yuetong Xia, Guangtong Xu, Langyou Wen, Guohua Gao, Baoning Zong. Hydrogen peroxide and applications in green hydrocarbon nitridation and oxidation [J]. Chinese Journal of Chemical Engineering, 2022, 41(1): 145-161.
[4]	Zhaohui Chen, Yasi Mo, Dong Lin, Yongxiao Tuo, Xiang Feng, Yibin Liu, Xiaobo Chen, De Chen, Chaohe Yang. Engineering the efficient three-dimension hollow cubic carbon from vacuum residuum with enhanced mass transfer ability towards H₂O₂ production [J]. Chinese Journal of Chemical Engineering, 2021, 38(10): 98-105.
[5]	Funing Sang, Jinpei Huang, Jianhong Xu. A circular microreaction method to the safe and efficient synthesis of 3-methylpyridine-N-oxide [J]. Chinese Journal of Chemical Engineering, 2020, 28(5): 1320-1325.
[6]	Guozhu Liu, Hairui Liang, Yajie Tian, Bofeng Zhang, Li Wang. Direct synthesis of hydrogen peroxide over Pd nanoparticles embedded between HZSM-5 nanosheets layers [J]. Chinese Journal of Chemical Engineering, 2020, 28(10): 2577-2586.
[7]	Wenjuan Yan, Wenxiang Zhang, Qi Xia, Shuaishuai Wang, Shuxia Zhang, Jian Shen, Xin Jin. Highly dispersed metal incorporated hexagonal mesoporous silicates for catalytic cyclohexanone oxidation to adipic acid [J]. Chinese Journal of Chemical Engineering, 2020, 28(10): 2542-2548.
[8]	Edgar N. Tec-Caamal, Refugio Rodríguez-Vázquez, Luis G. Torres-Bustillos, Ricardo Aguilar-López. Kinetic analysis via mathematical modeling for ferrous iron oxidation in a class of SBR-type system [J]. Chinese Journal of Chemical Engineering, 2019, 27(10): 2472-2480.
[9]	Xue Kang, Xiaoxun Ma, Jian'an Yin, Xuchun Gao. A study on simultaneous removal of NO and SO₂ by using sodium persulfate aqueous scrubbing [J]. Chin.J.Chem.Eng., 2018, 26(7): 1536-1544.
[10]	Xin Shi, Enxian Yuan, Guozhu Liu, Li Wang. Effects of porous oxide layer on performance of Pd-based monolithic catalysts for 2-ethylanthraquinone hydrogenation [J]. Chin.J.Chem.Eng., 2016, 24(11): 1570-1576.
[11]	LU Yiyu, LIU Yong, XIA Binwei, ZUO Weiqin. Phenol Oxidation by Combined Cavitation Water Jet and Hydrogen Peroxide [J]. Chin.J.Chem.Eng., 2012, 20(4): 760-767.
[12]	LI Wenjun, WU Di, SHI Xin, WEN Lixiong, SHAO Lei. Removal of Organic Matter and Ammonia Nitrogen in Azodicarbonamide Wastewater by a Combination of Power Ultrasound Radiation and Hydrogen Peroxide [J]. Chin.J.Chem.Eng., 2012, 20(4): 754-759.
[13]	CAI Weiquan, LI Huiquan, ZHANG Guangxu. Enhancement on Synthesis of Boehmite Through a Precarbonization-assisted Hydrogen Peroxide Route in Highly Alkaline Sodium Aluminate Solutions [J]. , 2010, 18(3): 500-505.
[14]	Asghar Molaei Dehkordi, Mohammad Amin Sobati, Mohammad Ali Nazem. Oxidative Desulfurization of Non-hydrotreated Kerosene Using Hydrogen Peroxide and Acetic Acid [J]. , 2009, 17(5): 869-874.
[15]	Tahir Imran QURESHI, Hong-Tae KIM, Young-Ju KIM. UV-Catalytic Treatment of Municipal Solid-Waste Landfill Leachate with Hydrogen Peroxide and Ozone Oxidation [J]. , 2002, 10(4): 444-449.