Distinct synergetic effects in the ozone enhanced photocatalytic degradation of phenol and oxalic acid with Fe3+/TiO2 catalyst

doi:10.1016/j.cjche.2018.01.017

Abstract

Abstract: In this work, phenol and oxalic acid (OA) degradation in an ozone and photocatalysis integrated process was intensively conducted with Fe³⁺/TiO₂ catalyst. The ferrioxalate complex formed between Fe³⁺ and oxalate accelerated the removal of OA in the ozonation, photolysis and photocatalytic ozonation process, for its high reactivity with ozone and UV. Phenol was degraded in ozonation and photolysis with limited TOC removal rates, but much higher TOC removal was achieved in photocatalytic ozonation due to the generation of·OH. The sequence of UV light and ozone in the sequential process also influences the TOC removal, and ozone is very powerful to oxidize intermediates catechol and hydroquinone to maleic acid. Fenton or photo-Fenton reactions only played a small part in Fe³⁺/TiO₂ catalyzed processes, because Fe³⁺ was greatly reduced but not regenerated in many cases. The synergetic effect was found to be highly related with the property of the target pollutants. Fe³⁺/TiO₂ catalyzed system showed the highest ability to destroy organics, but the TiO₂ catalyzed system showed little higher synergy.

Key words: Catalysis, Environment, Waste water, Fe³⁺/TiO₂, Synergistic effect, Photocatalytic ozonation

摘要： In this work, phenol and oxalic acid (OA) degradation in an ozone and photocatalysis integrated process was intensively conducted with Fe³⁺/TiO₂ catalyst. The ferrioxalate complex formed between Fe³⁺ and oxalate accelerated the removal of OA in the ozonation, photolysis and photocatalytic ozonation process, for its high reactivity with ozone and UV. Phenol was degraded in ozonation and photolysis with limited TOC removal rates, but much higher TOC removal was achieved in photocatalytic ozonation due to the generation of·OH. The sequence of UV light and ozone in the sequential process also influences the TOC removal, and ozone is very powerful to oxidize intermediates catechol and hydroquinone to maleic acid. Fenton or photo-Fenton reactions only played a small part in Fe³⁺/TiO₂ catalyzed processes, because Fe³⁺ was greatly reduced but not regenerated in many cases. The synergetic effect was found to be highly related with the property of the target pollutants. Fe³⁺/TiO₂ catalyzed system showed the highest ability to destroy organics, but the TiO₂ catalyzed system showed little higher synergy.

关键词: Catalysis, Environment, Waste water, Fe³⁺/TiO₂, Synergistic effect, Photocatalytic ozonation

Yongbing Xie, Yingying Chen, Jin Yang, Chenming Liu, He Zhao, Hongbin Cao. Distinct synergetic effects in the ozone enhanced photocatalytic degradation of phenol and oxalic acid with Fe³⁺/TiO₂ catalyst[J]. Chin.J.Chem.Eng., 2018, 26(7): 1528-1535.

References

[1] M.N. Chong, B. Jin, C.W.K. Chow, C. Saint, Recent developments in photocatalytic water treatment technology:A review, Water Res. 44(2010) 2997-3027.

[2] L.K. Putri, W.J. Ong, W.S. Chang, S.P. Chai, Heteroatom doped graphene in photocatalysis:A review, Appl. Surf. Sci. 358(2015) 2-14.

[3] X.M. Zhou, G. Liu, J.G. Yu, W.H. Fan, Surface plasmon resonance-mediated photocatalysis by noble metal-based composites under visible light, J. Mater. Chem. 22(2012) 21337-21354.

[4] M.R. Hoffmann, S.T. Martin, W.Y. Choi, D.W. Bahnemann, Environmental applications of semiconductor photocatalysis, Chem. Rev. 95(1995) 69-96.

[5] R. Asahi, T. Morikawa, T. Ohwaki, K. Aoki, Y. Taga, Visible-light photocatalysis in nitrogen-doped titanium oxides, Science 293(2001) 269-271.

[6] L. Pan, J.J. Zou, X.W. Zhang, L. Wang, Water-mediated promotion of dye sensitization of TiO₂ under visible light, J. Am. Chem. Soc. 133(2011) 10000-10002.

[7] K. Wang, Q. Li, B.S. Liu, B. Cheng, W.K. Ho, J.G. Yu, Sulfur-doped g-C₃N₄ with enhanced photocatalytic CO₂-reduction performance, Appl. Catal. B Environ. 176(2015) 44-52.

[8] Y. Kang, Y. Yang, L.C. Yin, X. Kang, L. Wang, G. Liu, H.M. Cheng, Selective breaking of hydrogen bonds of layered carbon nitride for visible light photocatalysis, Adv. Mater. 28(2016) 6471-6477.

[9] N. Zhang, C. Chen, Z. Mei, X. Liu, X. Qu, Y. Li, S. Li, W. Qi, Y. Zhang, J. Ye, V.A. Roy, R. Ma, Monoclinic tungsten oxide with {100} facet orientation and tuned electronic band structure for enhanced photocatalytic oxidations, ACS Appl. Mater. Interfaces 8(2016) 10367-10374.

[10] X.F. Zhu, B. Cheng, J.G. Yu, W.K. Ho, Halogen poisoning effect of Pt-TiO₂ for formaldehyde catalytic oxidation performance at room temperature, Appl. Surf. Sci. 364(2016) 808-814.

[11] H.Q. Sun, R. Ullah, S. Chong, H.M. Ang, M.O. Tade, S.B. Wang, Room-light-induced indoor air purification using an efficient Pt/N-TiO₂ photocatalyst, Appl. Catal. B Environ. 108-109(2011) 127-133.

[12] B.F. Xin, Z.Y. Ren, P. Wang, J. Liu, L.Q. Jing, H.G. Fu, Study on the mechanisms of photoinduced carriers separation and recombination for Fe³⁺-TiO₂ photocatalysts, Appl. Surf. Sci. 253(2007) 4390-4395.

[13] Y.Y. Chen, Y.B. Xie, J. Yang, H.B. Cao, Y. Zhang, Reaction mechanism and metal ion transformation in photocatalytic ozonation of phenol and oxalic acid with Ag⁺/TiO₂, J. Environ. Sci. 26(2014) 662-672.

[14] E. Piera, J.C. Calpe, E. Brillas, X. Domenech, J. Peral, 2,4-Dichlorophenoxyacetic acid degradation by catalyzed ozonation:TiO₂/UVA/O₃ and Fe(Ⅱ)/UVA/O₃ systems, Appl. Catal. B Environ. 27(2000) 169-177.

[15] U. von Gunten, Ozonation of drinking water:Part I. Oxidation kinetics and product formation, Water Res. 37(2003) 1443-1467.

[16] S. Esplugas, D.M. Bila, L.G.T. Krause, M. Dezotti, Ozonation and advanced oxidation technologies to remove endocrine disrupting chemicals (EDCs) and pharmaceuticals and personal care products (PPCPs) in water effluents, J. Hazard. Mater. 149(2007) 631-642.

[17] J.D. Xiao, Y.B. Xie, H.B. Cao, Organic pollutants removal in wastewater by heterogeneous photocatalytic ozonation, Chemosphere 121(2015) 1-17.

[18] F.J. Beltran, A. Almudena, F.G.A. Juan, Kinetic modelling of TOC removal in the photocatalytic ozonation of diclofenac aqueous solutions, Appl. Catal. B Environ. 100(2010) 289-298.

[19] F.J. Beltran, A. Aguinaco, J.F. Garcia-Araya, Mechanism and kinetics of sulfamethoxazole photocatalytic ozonation in water, Water Res. 43(2009) 1359-1369.

[20] J.D. Xiao, Y.B. Xie, H.B. Cao, Y.X. Wang, G. Zhuang, Y. Chen, Towards effective design of active nanocarbon materials for integrating visible-light photocatalysis with ozonation, Carbon 107(2016) 658-666.

[21] G.Z. Liao, D.Y. Zhu, L.S. Li, B.Y. Lan, Enhanced photocatalytic ozonation of organics by g-C₃N₄ under visible light irradiation, J. Hazard. Mater. 280(2014) 531-535.

[22] J. Xiao, Y. Xie, F. Nawaz, Y. Wang, P. Du, H. Cao, Dramatic coupling of visible light with ozone on honeycomb-like porous g-C₃N₄ towards superior oxidation of water pollutants, Appl. Catal. B Environ. 183(2016) 417-425.

[23] Y. Jing, L.S. Li, Q.Y. Zhang, P. Lu, P.H. Liu, X.H. Lu, Photocatalytic ozonation of dimethyl phthalate with TiO₂ prepared by a hydrothermal method, J. Hazard. Mater. 189(2011) 40-47.

[24] E. Mena, A. Rey, S. Contreras, F.J. Beltran, Visible light photocatalytic ozonation of DEET in the presence of different forms of WO₃, Catal. Today 252(2015) 100-106.

[25] S. Anandan, G.J. Lee, P.K. Chen, C.H. Fan, J.J. Wu, Removal of orange Ⅱ dye in water by visible light assisted photocatalytic ozonation using Bi₂O₃ and Au/Bi₂O₃ nanorods, Ind. Eng. Chem. Res. 49(2010) 9729-9737.

[26] H. Bader, J. Hoigne, Determination of ozone in water by the indigo method, Water Res. 15(1981) 449-456.

[27] H. Bader, V. Sturzenegger, J. Hoigne, Photometric-method for the determination of low concentrations of hydrogen peroxide by the peroxidase catalyzed oxidation of N,N-diethyl-p-phenylenediamine (DPD), Water Res. 22(1988) 1109-1115.

[28] R. Sauleda, E. Brillas, Mineralization of aniline and 4-chlorophenol in acidic solution by ozonation catalyzed with Fe²⁺ and UVA light, Appl. Catal. B Environ. 29(2001) 135-145.

[29] A. SafarzadehAmiri, J.R. Bolton, S.R. Cater, Ferrioxalate-mediated photodegradation of organic pollutants in contaminated water, Water Res. 31(1997) 787-798.

[30] E.M. Rodriguez, G. Fernandez, P.M. Alvarez, F.J. Beltran, TiO₂ and Fe (Ⅲ) photocatalytic ozonation processes of a mixture of emergent contaminants of water, Water Res. 46(2012) 152-166.

[31] F.J. Beltran, F.J. Rivas, R. Montero-de-Espinosa, Iron type catalysts for the ozonation of oxalic acid in water, Water Res. 39(2005) 3553-3564.

[32] L. Sanchez, J. Peral, X. Domenech, Aniline degradation by combined photocatalysis and ozonation, Appl. Catal. B Environ. 19(1998) 59-65.

[33] U. Cernigoj, U.L. Stangar, P. Trebse, Degradation of neonicotinoid insecticides by different advanced oxidation processes and studying the effect of ozone on TiO₂ photocatalysis, Appl. Catal. B Environ. 75(2007) 229-238.

[34] Y. Yamamoto, E. Niki, H. Shiokawa, Y. Kamiya, Ozonation of organic-compounds. 2. Ozonation of phenol in water, J. Org. Chem. 44(1979) 2137-2141.

[35] A.N.A. Arias, E. Arriola, J.R. Calle, E.B. Mesa, G.F. Zurita, Ethylene glycol mineralization by ferrioxalate-induced photo-Fenton, Rev. Int. Contam. Ambient. 32(2016) 213-226.

[36] J.Y. Fang, H.L. Liu, C.I. Shang, M.Z. Zeng, M.L. Ni, E. coli and bacteriophage MS₂ disinfection by UV, ozone and the combined UV and ozone processes, Front. Environ. Sci. Eng. 8(2013) 547-552.

[37] H. Sun, M. Sun, Y. Zhang, X. Quan, Catalytic ozonation of reactive red X-3B in aqueous solution under low pressure:Decolorization and OH·generation, Front. Environ. Sci. Eng. 9(2014) 591-595.

[38] R.A. Torres, J.I. Nieto, E. Combet, C. Petrier, C. Pulgarin, Influence of TiO₂ concentration on the synergistic effect between photocatalysis and high-frequency ultrasound for organic pollutant mineralization in water, Appl. Catal. B Environ. 80(2008) 168-175.

Distinct synergetic effects in the ozone enhanced photocatalytic degradation of phenol and oxalic acid with Fe³⁺/TiO₂ catalyst

Distinct synergetic effects in the ozone enhanced photocatalytic degradation of phenol and oxalic acid with Fe³⁺/TiO₂ catalyst

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Baoyu Liu, Feng Xiong, Jianwen Zhang, Manna Wang, Yi Huang, Yanxiong Fang, Jinxiang Dong. Enhanced ortho-selective t–butylation of phenol over sulfonic acid functionalized mesopore MTW zeolites [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 1-7.
[2]	Bo Yu, Guang Fu, Xinpei Li, Libo Zhang, Jing Li, Hongtao Qu, Dongbin Wang, Qingfeng Dong, Mengmeng Zhang. Arsenic removal from acidic industrial wastewater by ultrasonic activated phosphorus pentasulfide [J]. Chinese Journal of Chemical Engineering, 2023, 60(8): 46-52.
[3]	Fei Li, Xuemei Wang, Pengze Zhang, Qinqin Wang, Mingyuan Zhu, Bin Dai. Nitrogen and phosphorus co-doped activated carbon induces high density Cu⁺ active center for acetylene hydrochlorination [J]. Chinese Journal of Chemical Engineering, 2023, 59(7): 193-199.
[4]	Tingjun Fu, Ran Wang, Kun Ren, Liangliang Zhang, Zhong Li. Intensified shape selectivity and alkylation reaction for the two-step conversion of methanol aromatization to p-xylene [J]. Chinese Journal of Chemical Engineering, 2023, 59(7): 240-250.
[5]	Wei Wang, Romain Lemaire, Ammar Bensakhria, Denis Luart. Thermogravimetric analysis and kinetic modeling of the co-pyrolysis of a bituminous coal and poplar wood [J]. Chinese Journal of Chemical Engineering, 2023, 58(6): 53-68.
[6]	Yanli Zhang, Zhengkun Hou, Dong Yao, Xiaomin Qiu, Hongru Zhang, Peizhe Cui, Yinglong Wang, Jun Gao, Zhaoyou Zhu, Limei Zhong. Energy, exergy, economic and environmental comprehensive analysis and multi-objective optimization of a sustainable zero liquid discharge integrated process for fixed-bed coal gasification wastewater [J]. Chinese Journal of Chemical Engineering, 2023, 58(6): 341-354.
[7]	Haodi Tan, Minjiao Yang, Yingquan Chen, Xu Chen, Francesco Fantozzi, Pietro Bartocci, Roman Tschentscher, Federica Barontini, Haiping Yang, Hanping Chen. Preparation of aromatic hydrocarbons from catalytic pyrolysis of digestate [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 1-9.
[8]	Linlin Su, Meijun Chen, Li Gong, Hua Yang, Chao Chen, Jun Wu, Ling Luo, Gang Yang, Lulu Long. Boost activation of peroxymonosulfate by iron doped K_2-xMn₈O₁₆: Mechanism and properties [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 88-97.
[9]	Chenyang Zhao, Yinhan Cheng, Guangfei Qu, Yongheng Yuan, Fenghui Wu, Ye Liu, Shan Liu, Junyan Li, Ping Ning. High-performance liquid-phase catalytic purification of phosphine in tail gas using Pd(II)/Cu(II) composite [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 98-108.
[10]	Jixiang Liu, Xin Zhou, Gengfei Yang, Hui Zhao, Zhibo Zhang, Xiang Feng, Hao Yan, Yibin Liu, Xiaobo Chen, Chaohe Yang. Conceptual carbon-reduction process design and quantitative sustainable assessment for concentrating high purity ethylene from wasted refinery gas [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 290-308.
[11]	Yuhan Zhu, Jia Wei, Jun Li. Decontamination of Cr(VI) from water using sewage sludge-derived biochar: Role of environmentally persistent free radicals [J]. Chinese Journal of Chemical Engineering, 2023, 56(4): 97-103.
[12]	Iltaf Khan, Chunjuan Wang, Shoaib Khan, Jinyin Chen, Aftab Khan, Sayyar Ali Shah, Aihua Yuan, Sohail Khan, Mehwish K. Butt, Humaira Asghar. Bio-capped and green synthesis of ZnO/g-C₃N₄ nanocomposites and its improved antibiotic and photocatalytic activities: An exceptional approach towards environmental remediation [J]. Chinese Journal of Chemical Engineering, 2023, 56(4): 215-224.
[13]	Juan Du, Aibing Chen, Senlin Hou, Xueqing Gao. Self-deposition for mesoporous carbon nanosheet with supercapacitor application [J]. Chinese Journal of Chemical Engineering, 2023, 55(3): 34-40.
[14]	Mengting Liu, Xuexue Dong, Zengjing Guo, Aihua Yuan, Shuying Gao, Fu Yang. Enabling tandem oxidation of benzene to benzenediol over integrated neighboring V-Cu oxides in mesoporous silica [J]. Chinese Journal of Chemical Engineering, 2023, 55(3): 236-245.
[15]	Qian Zhu, Yan Zhuang, Hongqing Zhao, Peng Zhan, Cong Ren, Changsheng Su, Wenqiang Ren, Jiawen Zhang, Di Cai, Peiyong Qin. 2,5-Diformylfuran production by photocatalytic selective oxidation of 5-hydroxymethylfurfural in water using MoS₂/CdIn₂S₄ flower-like heterojunctions [J]. Chinese Journal of Chemical Engineering, 2023, 54(2): 180-191.