Citation: Ning Liu, Man Tian, Ye Zhang, Jinming Yang, Zhihao Wang, Wangxi Dai, Guixiang Quan, Jianqiu Lei, Xiaodong Zhang, Liang Tang. Three-dimensional MIL-88A(Fe)-derived α-Fe₂O₃ and graphene composite for efficient photo-Fenton-like degradation of ciprofloxacin[J]. Chinese Chemical Letters, ;2025, 36(12): 111063. doi: 10.1016/j.cclet.2025.111063 shu

Three-dimensional MIL-88A(Fe)-derived α-Fe₂O₃ and graphene composite for efficient photo-Fenton-like degradation of ciprofloxacin

Ning Liu ^a ,
Man Tian ^a ,
Ye Zhang ^a ,
Jinming Yang ^a ,
Zhihao Wang ^a ,
Wangxi Dai ^a ,
Guixiang Quan ^d ,
Jianqiu Lei ^c ,
Xiaodong Zhang ^{a, *,} ,
Liang Tang ^{b, *,}

a.
School of Environment and Architecture, University of Shanghai for Science and Technology, Shanghai 200093, China
b.
Key Laboratory of Organic Compound Pollution Control Engineering (MOE), School of Environmental and Chemical Engineering, Shanghai University, Shanghai 200444, China
c.
Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, China
d.
School of Environmental Science and Engineering, Yancheng Institute of Technology, Yancheng 224051, China

fatzhxd@126.com

tang1liang@shu.edu.cn

Received Date: 20 November 2024
Revised Date: 2 February 2025
Accepted Date: 10 March 2025
Available Online: 10 March 2025

Figures(5)

The photo-assisted Fenton-like method is an effective and sustainable way to remove organic pollutants from water. Herein, a series of three-dimensional composites containing MIL-88A(Fe)-derived α-Fe₂O₃ and graphene aerogel (GA-Fe-X) were designed and used as catalysts to degrade ciprofloxacin (CIP) by peroxymonosulfate (PMS) activated photo-Fenton-like technology. The as-prepared GA-Fe-1 displayed remarkable enhancement with a CIP degradation rate constant (0.017 min⁻¹) higher than that of graphene aerogel (0.0031 min⁻¹) and MIL-88A(Fe) (0.0039 min⁻¹). Experimental results demonstrated that the combination of MIL-88A(Fe)-derived α-Fe₂O₃ and graphene aerogel forming GA-Fe-X enhanced the separation efficiency of electron-hole pairs, activating PMS to produce SO₄^•−, ^•OH and ¹O₂ for enhanced CIP degradation through radical and non-radical pathways. The factors affecting CIP degradation during the photo-Fenton-like process were thoroughly investigated. The possible CIP degradation pathways and ecotoxicity of the intermediates were also analyzed. This work enhances our understanding of the photo-Fenton-like effect in three-dimensional graphene aerogel composites.
- Photo-Fenton-like,
- Peroxymonosulfate activation,
- Graphene aerogel,
- MIL-88A(Fe)-derived α-Fe₂O₃,
- Ciprofloxacin
1. [1]
  L. Perez-Bou, A. Gonzalez-Martinez, J. Gonzalez-Lopez, et al., Environ. Pollut. 342 (2024) 123115. doi: 10.1016/j.envpol.2023.123115
2. [2]
  T. Fayaz, N. Renuka. S.K. Ratha, Chemosphere 349 (2024) 140822. doi: 10.1016/j.chemosphere.2023.140822
3. [3]
  G.F. Zhang, X. Liu, S. Zhang, et al., Eur. J. Med. Chem. 146 (2018) 599–612. doi: 10.1016/j.ejmech.2018.01.078
4. [4]
  K. Wang, D. Gao, J. Xu, et al., Environ. Sci. Pollut. Res. Int. 25 (35) (2018) 35064–35073. doi: 10.1007/s11356-018-3413-0
5. [5]
  S. Ghosh, S. Pourebrahimi, A. Malloum, et al., Mater. Today Commun. 37 (2023) 107500. doi: 10.1016/j.mtcomm.2023.107500
6. [6]
  K. Sathishkumar, S. Naraginti, K. Lavanya, et al., Environ. Res. 235 (2023) 116558. doi: 10.1016/j.envres.2023.116558
7. [7]
  N.A. Alygizakis, P. Gago-Ferrero, V.L. Borova, et al., Sci. Total. Environ. 541 (2016) 1097–1105. doi: 10.1016/j.scitotenv.2015.09.145
8. [8]
  J. Qi, G. Jiang, Y. Wan, et al., Chem. Eng. J. 466 (2023) 142960. doi: 10.1016/j.cej.2023.142960
9. [9]
  Y. Yang, J. Ye, Y. Zhai, et al., Surf. Interfaces. 51 (2024) 104713. doi: 10.1016/j.surfin.2024.104713
10. [10]
  S. Wang J. Wang, Chem. Eng. J. 456 (2023) 141086. doi: 10.1016/j.cej.2022.141086
11. [11]
  N. Liu, J.L. Wang, M. Tian, et al., J. Colloid. Interface Sci. 603 (2021) 270–281. doi: 10.1016/j.jcis.2021.06.082
12. [12]
  H. He, Y. Wang, J. Li, et al., Chem. Eng. J. 427 (2022) 131962. doi: 10.1016/j.cej.2021.131962
13. [13]
  N. Liu, W.X. Dai, F.H. Fei, et al., Sep. Purif. Technol. 297 (2022) 121545. doi: 10.1016/j.seppur.2022.121545
14. [14]
  H. Deng, Y. Hui, C. Zhang, et al., Chin. Chem. Lett. 35 (6) (2024) 109078. doi: 10.1016/j.cclet.2023.109078
15. [15]
  X. Ma, H. Du, M. Tan, et al., Sep. Purif. Technol. 339 (2024) 126644. doi: 10.1016/j.seppur.2024.126644
16. [16]
  L. Jing, Y. Xu, M. Xie, et al., J. Colloid. Interface Sci. 659 (2024) 520–532. doi: 10.1016/j.jcis.2024.01.011
17. [17]
  H. Zhang, M. Li, J. Cao, et al., Ceram. Int. 44 (2018) 19958–19962. doi: 10.1016/j.ceramint.2018.07.262
18. [18]
  M. Farbod. M. Madadi Jaberi, Fuller Nanotub. Car. N. 29 (2021) 244–250. doi: 10.1080/1536383x.2020.1832995
19. [19]
  N. Liu, D.H. Wang, J.W. Xu, et al., Surf. Interfaces. 46 (2024) 104192. doi: 10.1016/j.surfin.2024.104192
20. [20]
  Q. Wang, H. Zhou, J. Qian, et al., J. Mater. Sci. Technol. 190 (2024) 67–75. doi: 10.1016/j.jmst.2023.11.045
21. [21]
  N. Liu, W.Y. Huang, X.D. Zhang, et al., Appl. Catal. B 221 (2018) 119–128. doi: 10.1016/j.apcatb.2017.09.020
22. [22]
  M. Tang, K. Tang, D. Wang, et al., Sep. Purif. Technol. 329 (2024) 125245. doi: 10.1016/j.seppur.2023.125245
23. [23]
  H. Wang, C. Zhang, L. Zheng, et al., J. Solid. State Chem. 323 (2023) 124051. doi: 10.1016/j.jssc.2023.124051
24. [24]
  Q. Xiang, H. Zhang, Z. Liu, et al., Chem. Eng. J. 480 (2024) 147825. doi: 10.1016/j.cej.2023.147825
25. [25]
  S.G. Khasevani. M.R. Gholami, Mater. Res. Bull. 106 (2018) 93–102. doi: 10.1016/j.materresbull.2018.05.024
26. [26]
  X.Y. Liao, F. Wang, F. Wang, et al., Appl. Catal. B 259 (2019) 118064. doi: 10.1016/j.apcatb.2019.118064
27. [27]
  Q. Ding, X.J. Zou, J. Ke, et al., J. Colloid. Interface Sci. 649 (2023) 148–158. doi: 10.1016/j.jcis.2023.06.095
28. [28]
  G. Sivakumari, M. Rajarajan, R. Naveenkumar, et al., Emergent. Mater. 6 (2023) 1243–1258. doi: 10.1007/s42247-023-00518-8
29. [29]
  X.L. Xu, W.H. Shi, P. Li, et al., Chem. Mater. 29 (2017) 6058–6065. doi: 10.1021/acs.chemmater.7b01947
30. [30]
  Q. Chen, J. Li, L. Cheng, et al., Chem. Eng. J. 379 (2020) 122389. doi: 10.1016/j.cej.2019.122389
31. [31]
  R. Ghasemzadeh. K. Akhbari, Inorg. Chem. 62 (2023) 17818–17829. doi: 10.1021/acs.inorgchem.3c02616
32. [32]
  M. Muschi. C. Serre, Coord. Chem. Rev. 387 (2019) 262–272. doi: 10.1016/j.ccr.2019.02.017
33. [33]
  Y. Fang, H. Wang, X. Wang, et al., Sep. Purif. Technol. 307 (2023) 122771. doi: 10.1016/j.seppur.2022.122771
34. [34]
  X. Zhang, J. Duan, Y. Tan, et al., Sep. Purif. Technol. 293 (2022) 121123. doi: 10.1016/j.seppur.2022.121123
35. [35]
  D. Li, H.M. Li, Q. Wen, et al., Adv. Funct. Mater. 34 (2024) 2313631. doi: 10.1002/adfm.202313631
36. [36]
  S.C. Ma, D. Yang, Y.A. Guan, et al., Appl. Catal. B 316 (2022) 121594. doi: 10.1016/j.apcatb.2022.121594
37. [37]
  H. Cheng, H. Liu, C. Huang, et al., Sep. Purif. Technol. 330 (2024) 125311. doi: 10.1016/j.seppur.2023.125311
38. [38]
  S.T. Li, L. Chang, K. Wang, et al., Chemosphere. 341 (2023) 140117-140117. doi: 10.1016/j.chemosphere.2023.140117
39. [39]
  J. Jiang, D. Shi, S. Niu, et al., J. Hazard. Mater. 468 (2024) 133749. doi: 10.1016/j.jhazmat.2024.133749
40. [40]
  K. Zhu, W. Qin, Y. Chen, et al., Nano Today. 58 (2024) 102462. doi: 10.1016/j.nantod.2024.102462
41. [41]
  Y. Huang, K. Zhu, Z. Hu, et al., J. Hazard. Mater. 466 (2024) 133611. doi: 10.1016/j.jhazmat.2024.133611
42. [42]
  N. Li, R. Li, X. Duan, et al., Environ. Sci. Technol. 55 (2021) 16163–16174. doi: 10.1021/acs.est.1c06244
43. [43]
  J. Sun, C. -H. Shen, J. Guo, et al., J. Colloid. Interface Sci. 588 (2021) 19–30. doi: 10.1016/j.jcis.2020.12.043
44. [44]
  F. Ye, Y. Su, R. Li, et al., Appl. Catal. B 337 (2023) 122992. doi: 10.1016/j.apcatb.2023.122992
45. [45]
  Q. Peng, X. Tang, K. Liu, et al., Minerals. 10 (2019) 10010002.
46. [46]
  T. Wang, C. Zhao, L. Meng, et al., Appl. Catal. B 334 (2023) 122832. doi: 10.1016/j.apcatb.2023.122832
47. [47]
  Y. Sun, X. Wang, Q. Fu, et al., ACS. Appl. Mater. Interfaces. 13 (33) (2021) 39331–39340. doi: 10.1021/acsami.1c09650
48. [48]
  Q. Wang, C. Zhang, R. Huo, et al., J. Environ. Manage 367 (2024) 122046. doi: 10.1016/j.jenvman.2024.122046
49. [49]
  Q. Wang, W. Ma, J. Qian, et al., Environ. Pollut. 347 (2024) 123707. doi: 10.1016/j.envpol.2024.123707
50. [50]
  W. Huo, M. Wang, H. Wei, et al., Appl. Surf. Sci. 639 (2023) 158199. doi: 10.1016/j.apsusc.2023.158199
51. [51]
  P.S. Bagus, C.J. Nelin, C.R. Brundle, et al., Phys. Chem. Chem. Phys. 24 (2022) 4562–4575. doi: 10.1039/d1cp04886d
52. [52]
  C. Yao, Z. Wang, Z. Xu, et al., J. Alloys. Compd. 941 (2023) 168920. doi: 10.1016/j.jallcom.2023.168920
53. [53]
  Z. Li, X. Yuan, H. Tang, et al., Environ. Sci. -Wat. Res. 8 (2022) 2744–2760. doi: 10.1039/d2ew00320a
54. [54]
  C. Liu, S. Mao, M. Shi, et al., J. Hazard. Mater. 420 (2021) 126613. doi: 10.1016/j.jhazmat.2021.126613
55. [55]
  F. Rong, Q. Lu, H. Mai, et al., ACS. Appl. Mater. Interfaces. 13 (2021) 21138–21148. doi: 10.1021/acsami.0c22825
56. [56]
  X. Jia, J. Zhang, Q. Huang, et al., Environ. Res. 241 (2024) 117639. doi: 10.1016/j.envres.2023.117639
57. [57]
  H. Mohebali, G. Moussavi, M. Karimi, et al., Sep. Purif. Technol. 315 (2023) 123670. doi: 10.1016/j.seppur.2023.123670
58. [58]
  Y. Wang, J. Chen, J. Gao, et al., Sep. Purif. Technol. 272 (2021) 118884. doi: 10.1016/j.seppur.2021.118884
59. [59]
  K.D. Jayeola, D.S. Sipuka, T.I. Sebokolodi, et al., Chem. Eng. J. 479 (2024) 147482. doi: 10.1016/j.cej.2023.147482
60. [60]
  Q. Man, F. Sun, Z. Zhang, et al., Sep. Purif. Technol. 349 (2024) 127915. doi: 10.1016/j.seppur.2024.127915
1. [1]
  Xian-Rui Meng , Qian Chen , Mei-Feng Wu , Qiang Wu , Su-Qin Wang , Li-Ping Jin , Fan Zhou , Ren-Li Ma , Jian-Ping Zou . Nano-flowers FeS/MoS2 composites as a peroxymonosulfate activator for efficient p-chlorophenol degradation. Chinese Journal of Structural Chemistry, 2025, 44(3): 100543-100543. doi: 10.1016/j.cjsc.2025.100543
2. [2]
  Hui Wang , Haodong Ji , Dandan Zhang , Xudong Yang , Hanchun Chen , Chunqian Jiang , Weiliang Sun , Jun Duan , Wen Liu . Solar-light-driven photocatalytic degradation and detoxification of ciprofloxacin using sodium niobate nanocubes decorated g-C₃N₄ with built-in electric field. Chinese Chemical Letters, 2025, 36(5): 110200-. doi: 10.1016/j.cclet.2024.110200
3. [3]
  Chunrui Zhao , Tianren Li , Jiage Li , Yansong Liu , Zian Fang , Xinyu Wang , Mingxin Huo , Shuangshi Dong , Mingyu Li . Doped cobalt for simultaneously promoting active (001) facet exposure of MIL-68(In) and acting as reactive sites in peroxymonosulfate-mediated photocatalytic decontamination. Chinese Chemical Letters, 2025, 36(5): 110201-. doi: 10.1016/j.cclet.2024.110201
4. [4]
  Lina Zou , Dengke Wang , Shiqin Lai , Xunheng Jiang , Siqi Chen , Lanqing Deng , Dong Fan , Hengshuai Li , Zhigang Zhou , Denglong Chen , Xiangyang Yao , Jianping Zou . Local spin-state manipulation of iron single-atom sites induced by sulfur modification to boost Fenton-like reaction. Chinese Chemical Letters, 2025, 36(12): 111094-. doi: 10.1016/j.cclet.2025.111094
5. [5]
  Cunjun Li , Wencong Liu , Xianlei Chen , Liang Li , Shenyu Lan , Mingshan Zhu . Adsorption and activation of peroxymonosulfate on BiOCl for carbamazepine degradation: The role of piezoelectric effect. Chinese Chemical Letters, 2024, 35(10): 109652-. doi: 10.1016/j.cclet.2024.109652
6. [6]
  Shifang Song , Chenyu Wu , Li Zhang , Dezhi Yang , Yang Lu , Zhengzheng Zhou . Unpacking phase transitions in multi-component drug systems: A case study. Chinese Chemical Letters, 2025, 36(7): 110911-. doi: 10.1016/j.cclet.2025.110911
7. [7]
  Cailiang Yue , Nan Sun , Yixing Qiu , Linlin Zhu , Zhiling Du , Fuqiang Liu . A direct Z-scheme 0D α-Fe₂O₃/TiO₂ heterojunction for enhanced photo-Fenton activity with low H₂O₂ consumption. Chinese Chemical Letters, 2024, 35(12): 109698-. doi: 10.1016/j.cclet.2024.109698
8. [8]
  Xun Zhu , Chenchen Zhang , Yingying Li , Yin Lu , Na Huang , Dawei Wang . Degradation of perfluorooctanoic acid by inductively heated Fenton-like process over the Fe₃O₄/MIL-101 composite. Chinese Chemical Letters, 2024, 35(12): 109753-. doi: 10.1016/j.cclet.2024.109753
9. [9]
  Jun Dong , Senyuan Tan , Sunbin Yang , Yalong Jiang , Ruxing Wang , Jian Ao , Zilun Chen , Chaohai Zhang , Qinyou An , Xiaoxing Zhang . Spatial confinement of free-standing graphene sponge enables excellent stability of conversion-type Fe₂O₃ anode for sodium storage. Chinese Chemical Letters, 2025, 36(3): 110010-. doi: 10.1016/j.cclet.2024.110010
10. [10]
  Xiangyang Ji , Yishuang Chen , Peng Zhang , Shaojia Song , Jian Liu , Weiyu Song . Boosting the first C–H bond activation of propane on rod-like V/CeO₂ catalyst by photo-assisted thermal catalysis. Chinese Chemical Letters, 2025, 36(5): 110719-. doi: 10.1016/j.cclet.2024.110719
11. [11]
  Aiping Liang , Chaolin Li , Chen Ling , Hengpan Duan , Wenhui Wang . CoTiO₃ for highly efficient peroxymonosulfate activation: The critical role of Co–O–Ti bond for rapid redox cycles of Co²⁺/Co³⁺. Chinese Chemical Letters, 2025, 36(10): 110788-. doi: 10.1016/j.cclet.2024.110788
12. [12]
  Mengxiang Zhu , Tao Ding , Yunzhang Li , Yuanjie Peng , Ruiping Liu , Quan Zou , Leilei Yang , Shenglei Sun , Pin Zhou , Guosheng Shi , Dongting Yue . Graphene controlled solid-state growth of oxygen vacancies riched V₂O₅ catalyst to highly activate Fenton-like reaction. Chinese Chemical Letters, 2024, 35(12): 109833-. doi: 10.1016/j.cclet.2024.109833
13. [13]
  Ruiying Liu , Li Zhao , Baishan Liu , Jiayuan Yu , Yujie Wang , Wanqiang Yu , Di Xin , Chaoqiong Fang , Xuchuan Jiang , Riming Hu , Hong Liu , Weijia Zhou . Modulating pollutant adsorption and peroxymonosulfate activation sites on Co3O4@N,O doped-carbon shell for boosting catalytic degradation activity. Chinese Journal of Structural Chemistry, 2024, 43(8): 100332-100332. doi: 10.1016/j.cjsc.2024.100332
14. [14]
  Tianjun Ni , Hui Zhang , Liping Zhou , Roujie Ma , Yanyu Wang , Zhijun Yang , Dan Luo , Nithima Khaorapapong , Xingtao Xu , Yusuke Yamauchi , Dong Liu . Atomic cobalt catalysts on 3D interconnected g-C₃N₄ support for activation of peroxymonosulfate: The importance of Co-N coordination effect. Chinese Chemical Letters, 2025, 36(9): 110659-. doi: 10.1016/j.cclet.2024.110659
15. [15]
  Yu Yao , Jinqiang Zhang , Yantao Wang , Kunsheng Hu , Yangyang Yang , Zhongshuai Zhu , Shuang Zhong , Huayang Zhang , Shaobin Wang , Xiaoguang Duan . Nitrogen-rich carbon for catalytic activation of peroxymonosulfate towards green synthesis. Chinese Chemical Letters, 2024, 35(11): 109633-. doi: 10.1016/j.cclet.2024.109633
16. [16]
  Ting Zhang , Baojing Huang , Hong Huang , Ailing Yan , Shiqiang Lu , Xufang Qian . Visible light boosted Fenton-like reaction of carbon dot-Fe(Ⅲ) complex: Kinetics and mechanism insights. Chinese Chemical Letters, 2025, 36(11): 110885-. doi: 10.1016/j.cclet.2025.110885
17. [17]
  Weichen Zhu , Wei Zuo , Pu Wang , Wei Zhan , Jun Zhang , Lipin Li , Yu Tian , Hong Qi , Rui Huang . Fe-N-C heterogeneous Fenton-like catalyst for the degradation of tetracycline: Fe-N coordination and mechanism studies. Chinese Chemical Letters, 2024, 35(9): 109341-. doi: 10.1016/j.cclet.2023.109341
18. [18]
  Qinwen Zheng , Xin Liu , Lintao Tian , Yi Zhou , Libing Liao , Guocheng Lv . Mechanism of Fenton catalytic degradation of Rhodamine B induced by microwave and Fe₃O₄. Chinese Chemical Letters, 2025, 36(4): 109771-. doi: 10.1016/j.cclet.2024.109771
19. [19]
  Haojie Duan , Hejingying Niu , Lina Gan , Xiaodi Duan , Shuo Shi , Li Li . Reinterpret the heterogeneous reaction of α-Fe₂O₃ and NO₂ with 2D-COS: The role of SDS, UV and SO₂. Chinese Chemical Letters, 2024, 35(6): 109038-. doi: 10.1016/j.cclet.2023.109038
20. [20]
  Gengchen Guo , Tianyu Zhao , Ruichang Sun , Mingzhe Song , Hongyu Liu , Sen Wang , Jingwen Li , Jingbin Zeng . Au-Fe₃O₄ dumbbell-like nanoparticles based lateral flow immunoassay for colorimetric and photothermal dual-mode detection of SARS-CoV-2 spike protein. Chinese Chemical Letters, 2024, 35(6): 109198-. doi: 10.1016/j.cclet.2023.109198

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(13)
HTML views(5)

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

Three-dimensional MIL-88A(Fe)-derived α-Fe2O3 and graphene composite for efficient photo-Fenton-like degradation of ciprofloxacin

Metrics

通讯作者: 陈斌, bchen63@163.com

Three-dimensional MIL-88A(Fe)-derived α-Fe₂O₃ and graphene composite for efficient photo-Fenton-like degradation of ciprofloxacin