Catalytic ozonation of thymol in reverse osmosis concentrate with core/shell Fe3O4@SiO2@Yb2O3 catalyst: Parameter optimization and degradation pathway

doi:10.1016/j.cjche.2016.10.017

Abstract

Abstract: In this work, a novel catalyst of Fe₃O₄@SiO₂@Yb₂O₃ was prepared and the degradation of thymol in reverse osmosis concentrate using ozonation was explored. The operational parameters, such as ozone dosage (8-48 mg·min^-1), initial thymol concentration (20-100 mg·L^-1), initial pH value (3-11), and catalyst Fe₃O₄@SiO₂@Yb₂O₃ dosage (0.2-1.0 g), were studied focusing on the thymol degradation and COD removal. The results indicated that the increase in ozone dosage, initial pH value, and Fe₃O₄@SiO₂@Yb₂O₃ dosage accelerated the thymol degradation and COD removal, while the increase in initial thymol concentration hampered the effect of ozonation. A pathway of thymol degradation by catalytic ozonation was proposed based on the intermediates detected by gas chromatography-mass spectrometer and ion chromatography. This paper can provide basic data and technical alternative for pollutant removal from reverse osmosis concentrate by ozonation.

Key words: Catalysis, Ozonation, Wastewater, Thymol, Degradation pathway

摘要： In this work, a novel catalyst of Fe₃O₄@SiO₂@Yb₂O₃ was prepared and the degradation of thymol in reverse osmosis concentrate using ozonation was explored. The operational parameters, such as ozone dosage (8-48 mg·min^-1), initial thymol concentration (20-100 mg·L^-1), initial pH value (3-11), and catalyst Fe₃O₄@SiO₂@Yb₂O₃ dosage (0.2-1.0 g), were studied focusing on the thymol degradation and COD removal. The results indicated that the increase in ozone dosage, initial pH value, and Fe₃O₄@SiO₂@Yb₂O₃ dosage accelerated the thymol degradation and COD removal, while the increase in initial thymol concentration hampered the effect of ozonation. A pathway of thymol degradation by catalytic ozonation was proposed based on the intermediates detected by gas chromatography-mass spectrometer and ion chromatography. This paper can provide basic data and technical alternative for pollutant removal from reverse osmosis concentrate by ozonation.

关键词: Catalysis, Ozonation, Wastewater, Thymol, Degradation pathway

Liang Wang, Anqi Liu, Zhaohui Zhang, Bin Zhao, Yingming Xia, Yun Tan. Catalytic ozonation of thymol in reverse osmosis concentrate with core/shell Fe₃O₄@SiO₂@Yb₂O₃ catalyst: Parameter optimization and degradation pathway[J]. , 2017, 25(5): 665-670.

References

[1] S.B. Grant, J.D. Saphores, D.L. Feldman, A.J. Hamilton, T.D. Fletcher, P.L.M. Cook, M. Stewardson, B.F. Sanders, L.A. Levin, R.F. Ambrose, A. Deletic, R. Brown, S.C. Jiang, D. Rosso, W.J. Cooper, I. Marusic, Taking the "waste" out of "wastewater" for human water security and ecosystem sustainability, Science 337(2012) 681-686.
[2] T.Y. Liu, C.K. Li, B. Pang, B. Van der Bruggen, X.L. Wang, Fabrication of a dual-layer (CA/PVDF) hollow fiber membrane for RO concentrate treatment, Desalination 365(2015) 57-69.
[3] S. Pradhan, L.H. Fan, F.A. Roddick, Removing organic and nitrogen content from a highly saline municipal wastewater reverse osmosis concentrate by UV/H₂O₂-BAC treatment, Chemosphere 136(2015) 198-203.
[4] Y.X. Sun, Y. Gao, H.Y. Hu, F. Tang, Z. Yang, Characterization and biotoxicity assessment of dissolved organic matter in RO concentrate from a municipal wastewater reclamation reverse osmosis system, Chemosphere 117(2014) 545-551.
[5] S. Malamis, E. Katsou, K. Takopoulos, P. Demetriou, M. Loizidou, Assessment of metal removal, biomass activity and RO concentrate treatment in an MBR-RO system, J. Hazard. Mater. 209(2012) 1-8.
[6] X.H. Lin, S.F.Y. Li, Determination of organic pollutants in municipal reverse osmosis concentrate by electrospray ionization-quadrupole time-of-flight tandem mass spectrometry and photocalaytic degradation methods, Desalination 344(2014) 206-211.
[7] A.M. Urtiaga, G. Perez, R. Ibanez, I. Ortiz, Removal of pharmaceuticals from a WWTP secondary effluent by ultrafiltration/reverse osmosis followed by electrochemical oxidation of the RO concentrate, Desalination 331(2013) 26-34.
[8] S. Ben Abdelmelek, J. Greaves, K.P. Ishida, W.J. Cooper, W.H. Song, Removal of pharmaceutical and personal care products from reverse osmosis retentate using advanced oxidation processes, Environ. Sci. Technol. 45(2011) 3665-3671.
[9] Y. Zhang, K. Ghyselbrecht, R. Vanherpe, B. Meesschaert, L. Pinoy, B. Van der Bruggen, RO concentrate minimization by electrodialysis:Techno-economic analysis and environmental concerns, J. Environ. Manag. 107(2012) 28-36.
[10] V. Hahn, K. Sunwoldt, A. Mikolasch, F. Schauer, Two different primary oxidation mechanisms during biotransformation of thymol by gram-positive bacteria of the genera Nocardia and Mycobacterium, Appl. Microbiol. Biotechnol. 97(2013) 1289-1297.
[11] N. Nakada, T. Tanishima, H. Shinohara, K. Kiri, H. Takada, Pharmaceutical chemicals and endocrine disrupters in municipal wastewater in Tokyo and their removal during activated sludge treatment, Water Res. 40(2006) 3297-3303.
[12] I. Tamura, K. Kagota, Y. Yasuda, S. Yoneda, J. Morita, N. Nakada, Y. Kameda, K. Kimura, N. Tatarazako, H. Yamamoto, Ecotoxicity and screening level ecotoxicological risk assessment of five antimicrobial agents:Triclosan, triclocarban, resorcinol, phenoxyethanol and p-thymol, J. Appl. Toxicol. 33(2013) 1222-1229.
[13] C.L. Eversloh, N. Henning, M. Schulz, T.A. Ternes, Electrochemical treatment of iopromide under conditions of reverse osmosis concentrates-Elucidation of the degradation pathway, Water Res. 48(2014) 237-246.
[14] L.F. Greenlee, B.D. Freeman, D.F. Lawler, Ozonation of phosphonate antiscalants used for reverse osmosis desalination:Parameter effects on the extent of oxidation, Chem. Eng. J. 244(2014) 505-513.
[15] A. Justo, O. Gonzalez, J. Acena, S. Perez, D. Barcelo, C. Sans, S. Esplugas, Pharmaceuticals and organic pollution mitigation in reclamation osmosis brines by UV/H₂O₂ and ozone, J. Hazard. Mater. 263(2013) 268-274.
[16] A.D. Coelho, C. Sans, A. Aguera, M.J. Gomez, S. Esplugas, M. Dezotti, Effects of ozone pre-treatment on diclofenac:Intermediates, biodegradability and toxicity assessment, Sci. Total Environ. 407(2009) 3572-3578.
[17] D.B. Mawhinney, B.J. Vanderford, S.A. Snyder, Transformation of 1H-benzotriazole by ozone in aqueous solution, Environ. Sci. Technol. 46(2012) 7102-7111.
[18] L. Zhao, J. Ma, Z.Z. Sun, X.D. Zhai, Mechanism of influence of initial pH on the degradation of nitrobenzene in aqueous solution by ceramic honeycomb catalytic ozonation, Environ. Sci. Technol. 42(2008) 4002-4007.
[19] Q.Z. Dai, L.L. Chen, W. Chen, J.M. Chen, Degradation and kinetics of phenoxyacetic acid in aqueous solution by ozonation, Sep. Purif. Technol. 142(2015) 287-292.
[20] T. Nothe, H. Fahlenkamp, C. von Sonntag, Ozonation of wastewater:Rate of ozone consumption and hydroxyl radical yield, Environ. Sci. Technol. 43(2009) 5990-5995.
[21] R. Rosal, A. Rodriguez, J.A. Perdigon-Melon, A. Petre, E. Garcia-Calvo, M.J. Gomez, A. Aguera, A.R. Fernandez-Alba, Degradation of caffeine and identification of the transformation products generated by ozonation, Chemosphere 74(2009) 825-831.
[22] M.J. Quero-Pastor, M.C. Garrido-Perez, A. Acevedo, J.M. Quiroga, Ozonation of ibuprofen:A degradation and toxicity study, Sci. Total Environ. 466(2014) 957-964.
[23] Z. Jeirani, A. Sadeghi, J. Soltan, B. Roshani, B. Rindall, Effectiveness of advanced oxidation processes for the removal of manganese and organic compounds in membrane concentrate, Sep. Purif. Technol. 149(2015) 110-115.
[24] J. Nawrocki, Catalytic ozonation in water:Controversies and questions. Discussion paper, Appl. Catal. B Environ. 142(2013) 465-471.
[25] H.Y. Ma, T.P. Spaniol, J. Okuda, Rare earth metal complexes supported by 1,omegadithiaalkanediyl-bridged, bis(phenolato) ligands:Synthesis, characterization and ring-opening polymerization catalysis of L-lactide, Dalton Trans. (2003) 4770-4780.
[26] Y.J. Feng, Y.H. Cui, B. Logan, Z.Q. Liu, Performance of Gd-doped Ti-based Sb-SnO₂ anodes for electrochemical destruction of phenol, Chemosphere 70(2008) 1629-1636.
[27] S. Bingham, W.A. Daoud, Recent advances in making nano-sized TiO₂ visible-light active through rare-earth metal doping, J. Mater. Chem. 21(2011) 2041-2050.
[28] Q.Y. Wang, G.F. Li, B. Zhao, M.Q. Shen, R.X. Zhou, The effect of La doping on the structure of Ce_0.2Zr_0.8O₂ and the catalytic performance of its supported Pd-only three-way catalyst, Appl. Catal. B Environ. 101(2010) 150-159.
[29] R.C. Martins, R.M. Quinta-Ferreira, Catalytic ozonation of phenolic acids over a Mn-Ce-O catalyst, Appl. Catal. B Environ. 90(2009) 268-277.
[30] M. Farbod, M. Kajbafvala, Effect of nanoparticle surface modification on the adsorption-enhanced photocatalysis of Gd/TiO₂ nanocomposite, Powder Technol. 239(2013) 434-440.
[31] Y.F. Ma, M.Y. Xing, J.L. Zhang, B.Z. Tian, F. Chen, Synthesis of well ordered mesoporous Yb, N co-doped TiO₂ with superior visible photocatalytic activity, Microporous Mesoporous Mater. 156(2012) 145-152.
[32] T. Sugimoto, E. Matijević, Formation of uniform spherical magnetite particles by crystallization from ferrous hydroxide gels, J. Colloid Interface Sci. 74(1980) 227-243.
[33] Q.Z. Dai, J.Y. Wang, J. Yu, J. Chen, J.M. Chen, Catalytic ozonation for the degradation of acetylsalicylic acid in aqueous solution by magnetic CeO₂ nanometer catalyst particles, Appl. Catal. B Environ. 144(2014) 686-693.
[34] T. Garoma, S. Matsumoto, Ozonation of aqueous solution containing bisphenol A:Effect of operational parameters, J. Hazard. Mater. 167(2009) 1185-1191.
[35] H.H. Yan, P. Lu, Z.Q. Pan, X. Wang, Q.Y. Zhang, L.S. Li, Ce/SBA-15 as a heterogeneous ozonation catalyst for efficient mineralization of dimethyl phthalate, J. Mol. Catal. A Chem. 377(2013) 57-64.
[36] M. Kuosa, J. Kallas, A. Häkkinen, Ozonation of p-nitrophenol at different pH values of water and the influence of radicals at acidic conditions, J. Environ. Chem. Eng. 3(2015) 325-332.
[37] J. Ma, M.H. Sui, T. Zhang, C.Y. Guan, Effect of pH on MnO_x/GAC catalyzed ozonation for degradation of nitrobenzene, Water Res. 39(2005) 779-786.
[38] L. Zhao, Z.Z. Sun, J. Ma, H.L. Liu, Enhancement mechanism of heterogeneous catalytic ozonation by cordierite-supported copper for the degradation of nitrobenzene in aqueous solution, Environ. Sci. Technol. 43(2009) 2047-2053.

Catalytic ozonation of thymol in reverse osmosis concentrate with core/shell Fe₃O₄@SiO₂@Yb₂O₃ catalyst: Parameter optimization and degradation pathway

Catalytic ozonation of thymol in reverse osmosis concentrate with core/shell Fe₃O₄@SiO₂@Yb₂O₃ catalyst: Parameter optimization and degradation pathway

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]	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.
[3]	Chaoyi Yin, Jingyuan Ma, Jian Qiu, Ruifang Liu, Long Ba. Mass-producible low-cost flexible electronic fabrics for azo dye wastewater treatment by electrocoagulation [J]. Chinese Journal of Chemical Engineering, 2023, 59(7): 222-230.
[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]	Chaozhi Zhang, Qianqian Shen, Yanxiao Su, Ruihua Jin. Efficient heavy metal recycling and water reuse from industrial wastewater using new reusable and inexpensive polyphenylene sulfide derivatives [J]. Chinese Journal of Chemical Engineering, 2023, 58(6): 89-102.
[6]	Chaobo Zhang, Xiaoyong Yang, Jian Dai, Wenxia Liu, Hang Yang, Zhishan Bai. Efficient extraction of phenol from wastewater by ionic micro-emulsion method: Anionic and cationic [J]. Chinese Journal of Chemical Engineering, 2023, 58(6): 137-145.
[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]	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.
[9]	Hu Chen, Ying Wang, Puyu Wang, Yongkang Lv. Assessing quinoline removal performances of an aerobic continuous moving bed biofilm reactor (MBBR) bioaugmented with Pseudomonas citronellolis LV1 [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 132-140.
[10]	Shichao Tian, Yuming Tu, Rujie Li, Yufan Du, Zhiyong Zhou, Fan Zhang, Zhongqi Ren. Comprehensive treatment of latex wastewater and resource utilization of concentrated liquid [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 183-192.
[11]	Yuxi Chai, Yanan Zhang, Yannan Tan, Zhiwei Li, Huangzhao Wei, Chenglin Sun, Haibo Jin, Zhao Mu, Lei Ma. Life cycle assessment of high concentration organic wastewater treatment by catalytic wet air oxidation [J]. Chinese Journal of Chemical Engineering, 2023, 56(4): 80-88.
[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.