Citation: Zhenzhong Liu, Siwen Wan, Yang Wu, Boyan Wang, Hongliang Ji. Highly Efficient Degradation of Sulfamethoxazole Using Activating Peracetic Acid with CoFe₂O₄/CuO[J]. Acta Physico-Chimica Sinica, ;2023, 39(5): 221101. doi: 10.3866/PKU.WHXB202211019 shu

Highly Efficient Degradation of Sulfamethoxazole Using Activating Peracetic Acid with CoFe₂O₄/CuO

1.
School of Resources and Environment, Nanchang University, Nanchang 330031, China
2.
School of Infrastructure Engineering, Nanchang University, Nanchang 330031, China

Corresponding author: Zhenzhong Liu, liuzz79@126.com
Received Date: 12 November 2022
Revised Date: 13 December 2022
Accepted Date: 14 December 2022
Available Online: 23 December 2022

Advanced oxidation processes (AOPs), especially AOPs that use transition metals as catalyst activated oxidants, are extremely effective in removing organic pollutants; they can completely degrade pollutants into CO₂ and H₂O. Thus, they have been widely studied in the field of water treatment. However, owing to the low catalytic efficiency and metal leakage, their applicability is currently limited. In this paper, the composite catalyst CoFe₂O₄/CuO containing spinel cobalt ferrite and copper oxide was successfully prepared by the chemical precipitation and sol-gel methods with two steps. The prepared CoFe₂O₄/CuO was characterized using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD), and its ability to remove sulfamethoxazole (SMX) with different AOPs was evaluated. Characterization results show that CoFe₂O₄ and CuO are well-complexed together, and the catalyst has good crystallinity. The effects of peracetic acid (PAA) concentration, catalyst dosage, common interfering substances (Cl⁻, HCO₃⁻, SO₄²⁻, and HA) in water, and different radical scavengers on SMX removal were also investigated. The results show that CoFe₂O₄/CuO has the characteristics of both CoFe₂O₄ and CuO. Compared with CoFe₂O₄ or CuO alone, CoFe₂O₄/CuO exhibits an excellent activation performance for PAA. Under the optimal reaction conditions (catalyst dosage = 20 mg·L⁻¹, c(PAA) = 200 μmol·L⁻¹, c(SMX) = 10 μmol·L⁻¹), the degradation rate of SMX reaches 92% within 90 s. The existence of Cu⁺/Cu²⁺ electron pairs can convert Co from the high valence to low valence state and accelerate the conversion of Co²⁺/Co³⁺, thereby improving the catalytic performance. An increase in the PAA concentration increases the removal efficiency of SMX; however, too high a concentration lowers removal efficiency. Compared to acidic or alkaline conditions, the CoFe₂O₄/CuO reaction system exhibits a better removal rate of SMX under neutral conditions. The common interfering substances in the environment have different effects on the CoFe₂O₄/CuO reaction system. Cl⁻ promotes the degradation of SMX by producing Cl•, HCO₃⁻ and HA inhibit the removal of SMX because of their quenching effect on free radicals, and SO₄²⁻ has no significant effect on the progress of the reaction. The XPS characterization results before and after the reaction show that the valence state of Co changes, indicating that Co is the main element involved in the activation of PAA. Radical quenching experiments demonstrate that the organic radical (R―O•) plays a dominant role in the removal of SMX. Further, the removal rate of SMX decreases after the catalyst is subjected to 3 recycle; nevertheless, it achieves a relatively rapid degradation of SMX (85% within 10 min).
- Spinel cobalt ferrite,
- Copper oxide,
- Advanced oxidation,
- Sulfamethoxazole,
- Peracetic acid,
- Organic radical
1. [1]
  Xie, Y.; Wan, J.; Yan, Z.; Wang, Y.; Xiao, T.; Hou, J.; Chen, H. Chem. Eng. J. 2022, 429, 132237. doi: 10.1016/j.cej.2021.132237 doi: 10.1016/j.cej.2021.132237
2. [2]
  Fu, J.; Feng, L.; Liu, Y.; Zhang, L.; Li, S. Chemosphere 2022, 287, 132094. doi: 10.1016/j.chemosphere.2021.132094 doi: 10.1016/j.chemosphere.2021.132094
3. [3]
  Zhu, W.; Sun, F.; Goei, R.; Zhou, Y. Appl. Catal. B 2017, 207, 93. doi: 10.1016/j.apcatb.2017.02.012 doi: 10.1016/j.apcatb.2017.02.012
4. [4]
  Nguyen, T.-B.; Huang, C.; Doong, R.-A.; Chen, C.-W.; Dong, C.-D. Chem. Eng. J. 2020, 384, 123383. doi: 10.1016/j.cej.2019.123383 doi: 10.1016/j.cej.2019.123383
5. [5]
  Wang, X.; Lu, W.; Zhao, Z.; Zhong, H.; Zhu, Z.; Chen, W. Chem. Eng. J. 2020, 400, 125872. doi: 10.1016/j.cej.2020.125872 doi: 10.1016/j.cej.2020.125872
6. [6]
  Kim, J.; Du, P.; Liu, W.; Luo, C.; Zhao, H.; Huang, C.-H. Environ. Sci. Technol. 2020, 54, 5268. doi: 10.1021/acs.est.0c00356 doi: 10.1021/acs.est.0c00356
7. [7]
  Luukkonen, T.; Heyninck, T.; Rämö, J.; Lassi, U. Water Res. 2015, 85, 275. doi: 10.1016/j.watres.2015.08.037 doi: 10.1016/j.watres.2015.08.037
8. [8]
  Henao, L. D.; Turolla, A.; Antonelli, M. Chemosphere 2018, 213, 25. doi: 10.1016/j.chemosphere.2018.09.005 doi: 10.1016/j.chemosphere.2018.09.005
9. [9]
  Zhou, X.; Wu, H.; Zhang, L.; Liang, B.; Sun, X.; Chen, J. Molecules 2020, 25, 2725. doi: 10.3390/molecules25122725 doi: 10.3390/molecules25122725
10. [10]
  Cai, M.; Sun, P.; Zhang, L.; Huang, C.-H. Environ. Sci. Technol. 2017, 51, 14217. doi: 10.1021/acs.est.7b04694 doi: 10.1021/acs.est.7b04694
11. [11]
  Chen, S.; Cai, M.; Liu, Y.; Zhang, L.; Feng, L. Water Res. 2019, 150, 153. doi: 10.1016/j.watres.2018.11.044 doi: 10.1016/j.watres.2018.11.044
12. [12]
  Li, W.; Li, Y.; Zhang, D.; Lan, Y.; Guo, J. J. Hazard. Mater. 2020, 381, 121209. doi: 10.1016/j.jhazmat.2019.121209 doi: 10.1016/j.jhazmat.2019.121209
13. [13]
  Cruz, D. R.; de Jesus, G. K.; Santos, C. A.; Silva, W. R.; Wisniewski, A., Jr.; Cunha, G. C.; Romão, L. P. Chemosphere 2021, 280, 130675. doi: 10.1016/j.chemosphere.2021.130675 doi: 10.1016/j.chemosphere.2021.130675
14. [14]
  Yu, J.; Qiu, W.; Xu, H.; Lu, X.; Ma, J.; Lu, D. Chem. Eng. J. 2021, 421, 129498. doi: 10.1016/j.cej.2021.129498 doi: 10.1016/j.cej.2021.129498
15. [15]
  Ding, R.-R.; Li, W.-Q.; He, C.-S.; Wang, Y.-R.; Liu, X.-C.; Zhou, G.-N.; Mu, Y. Appl. Catal. B 2021, 291, 120069. doi: 10.1016/j.apcatb.2021.120069 doi: 10.1016/j.apcatb.2021.120069
16. [16]
  Hasanvandian, F.; Shokri, A.; Moradi, M.; Kakavandi, B.; Setayesh, S. R. J. Hazard. Mater. 2022, 423, 127090. doi: 10.1016/j.jhazmat.2021.127090 doi: 10.1016/j.jhazmat.2021.127090
17. [17]
  Xiong, W.-H.; Zhang, W.-C.; Yu, C.-P.; Shen, R.-Q.; Cheng, J.; Ye, J.-H.; Qin, Z.-C. Acta Phys. -Chim. Sin. 2016, 32, 2093. doi: 10.3866/PKU.WHXB201605121
18. [18]
  Ren, Y.; Lin, L.; Ma, J.; Yang, J.; Feng, J.; Fan, Z. Appl. Catal. B 2015, 165, 572. doi: 10.1016/j.apcatb.2014.10.051 doi: 10.1016/j.apcatb.2014.10.051
19. [19]
  Guan, Y.-H.; Ma, J.; Ren, Y.-M.; Liu, Y.-L.; Xiao, J.-Y.; Lin, L.-Q.; Zhang, C. Water Res. 2013, 47, 5431. doi: 10.1016/j.watres.2013.06.023 doi: 10.1016/j.watres.2013.06.023
20. [20]
  Chen, X.-L.; Li, F.; Zhang, M.; Liu, B.; Chen, H.; Wang, H. Sci. Total Environ. 2021, 777, 145794. doi: 10.1016/j.scitotenv.2021.145794 doi: 10.1016/j.scitotenv.2021.145794
21. [21]
  Chu, S.; Li, X.; W. Robertson, A.; Sun, Z. Acta Phys. -Chim. Sin. 2021, 37, 2009023. doi: 10.3866/PKU.WHXB202009023
22. [22]
  Wang, M.; Jin, C.; Kang, J.; Liu, J.; Tang, Y.; Li, Z.; Li, S. Chem. Eng. J. 2021, 416, 128118. doi: 10.1016/j.cej.2020.128118 doi: 10.1016/j.cej.2020.128118
23. [23]
  Kiani, R.; Mirzaei, F.; Ghanbari, F.; Feizi, R.; Mehdipour, F. J. Water Process Eng. 2020, 38, 101623. doi: 10.1016/j.jwpe.2020.101623 doi: 10.1016/j.jwpe.2020.101623
24. [24]
  Zhou, J.-J.; Ji, W.; Xu, L.; Yang, Y.; Wang, W.; Ding, H.; Xu, X.; Wang, W.; Zhang, P.; Hua, Z. Chem. Eng. J. 2022, 428, 132123. doi: 10.1016/j.cej.2021.132123 doi: 10.1016/j.cej.2021.132123
25. [25]
  Yu, R.; Zhao, J.; Zhao, Z.; Cui, F. J. Hazard. Mater. 2020, 390, 121998. doi: 10.1016/j.jhazmat.2019.121998 doi: 10.1016/j.jhazmat.2019.121998
26. [26]
  Lin, J.-Y.; Chen, P.-Y.; Kwon, E.; Da Oh, W.; You, S.; Huang, C.-W.; Ghanbari, F.; Wi-Afedzi, T.; Lin, K.-Y. A. J. Water Process Eng. 2021, 40, 101933. doi: 10.1016/j.jwpe.2021.101933 doi: 10.1016/j.jwpe.2021.101933
27. [27]
  Li, Y.; Zhu, W.; Guo, Q.; Wang, X.; Zhang, L.; Gao, X.; Luo, Y. Sep. Purif. Technol. 2021, 276. doi: 10.1016/j.seppur.2021.119403 doi: 10.1016/j.seppur.2021.119403
28. [28]
  Wang, J.; Xiong, B.; Miao, L.; Wang, S.; Xie, P.; Wang, Z.; Ma, J. Appl. Catal. B 2021, 280, 119422. doi: 10.1016/j.apcatb.2020.119422 doi: 10.1016/j.apcatb.2020.119422
29. [29]
  Zhang, P.; Zhang, X.; Zhao, X.; Jing, G.; Zhou, Z. J. Hazard. Mater. 2022, 424, 127653. doi: 10.1016/j.jhazmat.2021.127653 doi: 10.1016/j.jhazmat.2021.127653
30. [30]
  Chen, C.; Liu, L.; Guo, J.; Zhou, L.; Lan, Y. Chem. Eng. J. 2019, 361, 1304. doi: 10.1016/j.cej.2018.12.156 doi: 10.1016/j.cej.2018.12.156
31. [31]
  Li, R.; Manoli, K.; Kim, J.; Feng, M.; Huang, C. H.; Sharma, V. K. Environ. Sci. Technol. 2021, 55, 9150. doi: 10.1021/acs.est.0c06676 doi: 10.1021/acs.est.0c06676
32. [32]
  Zhang, L.; Chen, J.; Zheng, T.; Xu, Y.; Liu, T.; Yin, W.; Zhang, Y.; Zhou, X. Water Res. 2022, 229, 119462. doi: 10.1016/j.watres.2022.119462 doi: 10.1016/j.watres.2022.119462
33. [33]
  Kim, J.; Zhang, T.; Liu, W.; Du, P.; Dobson, J. T.; Huang, C.-H. Environ. Sci. Technol. 2019, 53, 13312. doi: 10.1021/acs.est.9b02991 doi: 10.1021/acs.est.9b02991
34. [34]
  Wu, W.; Tian, D.; Liu, T.; Chen, J.; Huang, T.; Zhou, X.; Zhang, Y. Chem. Eng. J. 2020, 394, 124938. doi: 10.1016/j.cej.2020.124938 doi: 10.1016/j.cej.2020.124938
35. [35]
  Dong, J.; Xu, W.; Liu, S.; Gong, Y.; Yang, T.; Du, L.; Chen, Q.; Tan, X.; Liu, Y. Chem. Eng. J. 2022, 430, 132868. doi: 10.1016/j.cej.2021.132868 doi: 10.1016/j.cej.2021.132868
36. [36]
  Liu, Y.; He, X.; Duan, X.; Fu, Y.; Dionysiou, D. D. Chem. Eng. J. 2015, 276, 113. doi: 10.1016/j.cej.2015.04.048 doi: 10.1016/j.cej.2015.04.048
37. [37]
  Hu, J.; Li, T.; Zhang, X.; Ren, H.; Huang, H. Chemosphere 2022, 287, 132261. doi: 10.1016/j.chemosphere.2021.132261 doi: 10.1016/j.chemosphere.2021.132261
38. [38]
  Wang, L.; Yan, T.; Tang, R.; Ping, Q.; Li, Y.; Wang, J. Water Res. 2021, 205, 117684. doi: 10.1016/j.watres.2021.117684 doi: 10.1016/j.watres.2021.117684
39. [39]
  Zhang, L.; Fu, Y.; Wang, Z.; Zhou, G.; Zhou, R.; Liu, Y. Sep. Purif. Technol. 2021, 276, 119319. doi: 10.1016/j.seppur.2021.119319 doi: 10.1016/j.seppur.2021.119319
40. [40]
  Hu, P.; Long, M. Appl. Catal. B 2016, 181, 103. doi: 10.1016/j.apcatb.2015.07.024 doi: 10.1016/j.apcatb.2015.07.024
41. [41]
  Chen, Y.; Liu, Y.; Zhang, L.; Xie, P.; Wang, Z.; Zhou, A.; Fang, Z.; Ma, J. J. Hazard. Mater. 2018, 353, 18. doi: 10.1016/j.jhazmat.2018.03.050 doi: 10.1016/j.jhazmat.2018.03.050
1. [1]
  Dan-Ying Xing , Xiao-Dan Zhao , Chuan-Shu He , Bo Lai . Kinetic study and DFT calculation on the tetracycline abatement by peracetic acid. Chinese Chemical Letters, 2024, 35(9): 109436-. doi: 10.1016/j.cclet.2023.109436
2. [2]
  Tianbo Jia , Lili Wang , Zhouhao Zhu , Baikang Zhu , Yingtang Zhou , Guoxing Zhu , Mingshan Zhu , Hengcong Tao . Modulating the degree of O vacancy defects to achieve selective control of electrochemical CO₂ reduction products. Chinese Chemical Letters, 2024, 35(5): 108692-. doi: 10.1016/j.cclet.2023.108692
3. [3]
  Yuxin Wang , Zhengxuan Song , Yutao Liu , Yang Chen , Jinping Li , Libo Li , Jia Yao . Methyl functionalization of trimesic acid in copper-based metal-organic framework for ammonia colorimetric sensing at high relative humidity. Chinese Chemical Letters, 2024, 35(6): 108779-. doi: 10.1016/j.cclet.2023.108779
4. [4]
  Zhengzhong Zhu , Shaojun Hu , Zhi Liu , Lipeng Zhou , Chongbin Tian , Qingfu Sun . A cationic radical lanthanide organic tetrahedron with remarkable coordination enhanced radical stability. Chinese Chemical Letters, 2025, 36(2): 109641-. doi: 10.1016/j.cclet.2024.109641
5. [5]
  Bing Jiang , Gang Zou , Bi Luo , Yan Guo , Jingru Li , Wendi Zhang , Qianxiao Fan , Lehao Liu , Lihua Chu , Qiaobao Zhang , Meicheng Li . Enhanced electrochemical performance of lithium-rich layered oxide materials: Exploring advanced coating strategies. Chinese Chemical Letters, 2025, 36(4): 109801-. doi: 10.1016/j.cclet.2024.109801
6. [6]
  Jing-Qi Tao , Shuai Liu , Tian-Yu Zhang , Hong Xin , Xu Yang , Xin-Hua Duan , Li-Na Guo . Photoinduced copper-catalyzed alkoxyl radical-triggered ring-expansion/aminocarbonylation cascade. Chinese Chemical Letters, 2024, 35(6): 109263-. doi: 10.1016/j.cclet.2023.109263
7. [7]
  Yu-Yu Tan , Lin-Heng He , Wei-Min He . Copper-mediated assembly of SO₂F group via radical fluorine-atom transfer strategy. Chinese Chemical Letters, 2024, 35(9): 109986-. doi: 10.1016/j.cclet.2024.109986
8. [8]
  Shili Wang , Mamitiana Roger Razanajatovo , Xuedong Du , Shunli Wan , Xin He , Qiuming Peng , Qingrui Zhang . Recent advances on decomplexation mechanisms of heavy metal complexes in persulfate-based advanced oxidation processes. Chinese Chemical Letters, 2024, 35(6): 109140-. doi: 10.1016/j.cclet.2023.109140
9. [9]
  Chu Wu , Zhichao Dong , Jinfang Hou , Jian Peng , Shuangyu Wu , Xiaofang Wang , Xiangwei Kong , Yue Jiang . Application of titanium-based advanced oxidation processes in pesticide-contaminated water purification: Emerging opportunities and challenges. Chinese Chemical Letters, 2025, 36(3): 110438-. doi: 10.1016/j.cclet.2024.110438
10. [10]
  Huijuan Li , Zhu Wang , Jiagen Geng , Ruiping Song , Xiaoyin Liu , Chaochen Fu , Si Li . Current advances in UV-based advanced oxidation processes for the abatement of fluoroquinolone antibiotics in wastewater. Chinese Chemical Letters, 2025, 36(4): 110138-. doi: 10.1016/j.cclet.2024.110138
11. [11]
  Xiaoling WANG , Hongwu ZHANG , Daofu LIU . Synthesis, structure, and magnetic property of a cobalt(Ⅱ) complex based on pyridyl-substituted imino nitroxide radical. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 407-412. doi: 10.11862/CJIC.20240214
12. [12]
  Qi Li , Zi-Lu Wang , Yun-He Xu . Copper-catalyzed 1,4-silylcyanation of 1,3-enynes: A silyl radical-initiated approach for synthesis of difunctionalized allenes. Chinese Chemical Letters, 2025, 36(3): 109991-. doi: 10.1016/j.cclet.2024.109991
13. [13]
  Jingtai Bi , Yupeng Cheng , Mengmeng Sun , Xiaofu Guo , Shizhao Wang , Yingying Zhao . Efficient and selective photocatalytic nitrite reduction to N₂ through CO₂ anion radical by eco-friendly tartaric acid activation. Chinese Chemical Letters, 2024, 35(11): 109639-. doi: 10.1016/j.cclet.2024.109639
14. [14]
  Hanqing Zhang , Xiaoxia Wang , Chen Chen , Xianfeng Yang , Chungli Dong , Yucheng Huang , Xiaoliang Zhao , Dongjiang Yang . Selective CO2-to-formic acid electrochemical conversion by modulating electronic environment of copper phthalocyanine with defective graphene. Chinese Journal of Structural Chemistry, 2023, 42(10): 100089-100089. doi: 10.1016/j.cjsc.2023.100089
15. [15]
  Wei Zhou , Xi Chen , Lin Lu , Xian-Rong Song , Mu-Jia Luo , Qiang Xiao . Recent advances in electrocatalytic generation of indole-derived radical cations and their applications in organic synthesis. Chinese Chemical Letters, 2024, 35(4): 108902-. doi: 10.1016/j.cclet.2023.108902
16. [16]
  Ling Fang , Sha Wang , Shun Lu , Fengjun Yin , Yujie Dai , Lin Chang , Hong Liu . Efficient electroreduction of nitrate via enriched active phases on copper-cobalt oxides. Chinese Chemical Letters, 2024, 35(4): 108864-. doi: 10.1016/j.cclet.2023.108864
17. [17]
  Fereshte Hassanzadeh-Afruzi , Mina Azizi , Iman Zare , Ehsan Nazarzadeh Zare , Anwarul Hasan , Siavash Iravani , Pooyan Makvandi , Yi Xu . Advanced metal-organic frameworks-polymer platforms for accelerated dermal wound healing. Chinese Chemical Letters, 2024, 35(11): 109564-. doi: 10.1016/j.cclet.2024.109564
18. [18]
  Shimei Wu , Yining Li , Lantao Chen , Yufei Zhang , Lingxing Zeng , Haosen Fan . Hexapod cobalt phosphosulfide nanorods encapsulating into multiple hetero-atom doped carbon frameworks for advanced sodium/potassium ion battery anodes. Chinese Chemical Letters, 2025, 36(4): 109796-. doi: 10.1016/j.cclet.2024.109796
19. [19]
  Muhammad Riaz , Rakesh Kumar Gupta , Di Sun , Mohammad Azam , Ping Cui . Selective adsorption of organic dyes and iodine by a two-dimensional cobalt(II) metal-organic framework. Chinese Journal of Structural Chemistry, 2024, 43(12): 100427-100427. doi: 10.1016/j.cjsc.2024.100427
20. [20]
  Mengmeng Ao , Jian Wei , Chuan-Shu He , Heng Zhang , Zhaokun Xiong , Yonghui Song , Bo Lai . Insight into the activation of peroxymonosulfate by N-doped copper-based carbon for efficient degradation of organic pollutants: Synergy of nonradicals. Chinese Chemical Letters, 2025, 36(1): 109882-. doi: 10.1016/j.cclet.2024.109882

Get Citation

PDF

XML

Metrics

PDF Downloads(4)
Abstract views(536)
HTML views(65)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Highly Efficient Degradation of Sulfamethoxazole Using Activating Peracetic Acid with CoFe2O4/CuO

Metrics

通讯作者: 陈斌, bchen63@163.com

Highly Efficient Degradation of Sulfamethoxazole Using Activating Peracetic Acid with CoFe₂O₄/CuO