Citation: Jian Peng, Yue Jiang, Shuangyu Wu, Yanran Cheng, Jingyu Liang, Yixin Wang, Zhuo Li, Sijie Lin. A nonradical oxidation process initiated by Ti-peroxo complex showed high specificity toward the degradation of tetracycline antibiotics[J]. Chinese Chemical Letters, ;2024, 35(5): 108903. doi: 10.1016/j.cclet.2023.108903 shu

A nonradical oxidation process initiated by Ti-peroxo complex showed high specificity toward the degradation of tetracycline antibiotics

Jian Peng ^{a, b, 1} ,
Yue Jiang ^{a, b, 1} ,
Shuangyu Wu ^{a, b} ,
Yanran Cheng ^{a, b} ,
Jingyu Liang ^{a, b} ,
Yixin Wang ^{a, b} ,
Zhuo Li ^b ,
Sijie Lin ^{a, b, *,}

a.
College of Environmental Science and Engineering, Biomedical Multidisciplinary Innovation Research Institute, Shanghai East Hospital, Tongji University, Shanghai 200092, China
b.
Key Laboratory of Yangtze River Water Environment, Shanghai Institute of Pollution Control and Ecological Security, Tongji University, Shanghai 200092, China

lin.sijie@tongji.edu.cn

Received Date: 22 April 2023
Revised Date: 17 July 2023
Accepted Date: 6 August 2023
Available Online: 9 August 2023

Figures(4)

Nonradical oxidation has received wide attention in advanced oxidation processes for environmental remediation. Understanding the relationship between material characteristics and their ability to initiate nonradical oxidation processes is the key to better material design and performance. Herein, a novel titanium-based metal-organic framework MIL-125-Ti/H₂O₂ system was established to show a highly selective degradation efficacy toward tetracycline antibiotics. MIL-125-Ti with the abundance of TiO₆ octahedra units was found to effectively activate H₂O₂ under dark conditions by forming an oxidative Ti-peroxo complex. The presence of the Ti-peroxo complex, confirmed by UV-visible spectrophotometer, fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy characterizations, showed superior degradation (> 95% removal rate) of oxytetracycline hydrochloride (OTC), doxycycline hydrochloride, chlortetracycline hydrochloride, and tetracycline. Density functional theory calculations were performed to assist the elucidation on the mechanism of H₂O₂ activation and antibiotics degradation. The MIL-125-Ti/H₂O₂ system was highly resistant to halogens and background organics, and could well maintain its original catalytic activity in actual water matrices. It retained the ability to degrade 75% of OTC within ten test cycles. This study provides new insight into the nonradical oxidation process initiated by the unique Ti-peroxo complex of Ti-based MOF.
- Nonradical oxidation,
- Metal-organic frameworks,
- Advanced oxidation process,
- Ti-peroxo complex,
- Antibiotics degradation
1. [1]
  F. Gozzo, J. Mol. Catal. A: Chem. 171 (2001) 1–22. doi: 10.1016/S1381-1169(01)00099-1
2. [2]
  Y. Jiang, D. Baimanov, S. Jin, et al., Proc. Natl. Acad. Sci. U. S. A. 120 (2023) e2210211120. doi: 10.1073/pnas.2210211120
3. [3]
  F.J. Rivas, F.J. Beltran, J. Frades, et al., Water Res. 35 (2001) 387–396. doi: 10.1016/S0043-1354(00)00285-2
4. [4]
  P.H. Shao, J.Y. Tian, F. Yang, et al., Adv. Funct. Mater. 28 (2018) 1705295. doi: 10.1002/adfm.201705295
5. [5]
  S.J. Ye, G.M. Zeng, X.F. Tan, et al., Appl. Catal. B: Environ. 269 (2020) 118850. doi: 10.1016/j.apcatb.2020.118850
6. [6]
  J.B. Chen, J. Xu, T.C. Liu, et al., J. Hazard. Mater. 386 (2020) 121656. doi: 10.1016/j.jhazmat.2019.121656
7. [7]
  M.M. Wang, Y.K. Cui, H.Y. Cao, et al., Appl. Catal. B: Environ. 282 (2021) 119585. doi: 10.1016/j.apcatb.2020.119585
8. [8]
  T. Zhang, Y. Chen, Y.R. Wang, et al., Environ. Sci. Technol. 48 (2014) 5868–5875. doi: 10.1021/es501218f
9. [9]
  Y. Bao, C. Lian, K. Huang, et al., Angew. Chem. Int. Ed. 61 (2022) e2022095.
10. [10]
  J. Song, Z. Huang, J. Mao, et al., Chem. Eng. J. 396 (2020) 125246. doi: 10.1016/j.cej.2020.125246
11. [11]
  M. Lin, C.J. Xia, B. Zhu, et al., Chem. Eng. J. 295 (2016) 370–375. doi: 10.1016/j.cej.2016.02.072
12. [12]
  M.G. Zuo, X.Q. Huang, J.X. Li, et al., Catal. Sci. Technol. 9 (2019) 2923–2930. doi: 10.1039/C9CY00298G
13. [13]
  X. Feng, D. Lin, D. Chen, et al., Sci. Bull. 66 (2021) 1945–1949. doi: 10.1016/j.scib.2021.05.020
14. [14]
  L. Xu, J.H. Ding, Y.L. Yang, et al., J. Catal. 309 (2014) 1–10. doi: 10.1016/j.jcat.2013.08.021
15. [15]
  Y. Wei, G. Li, R.M. Su, et al., Appl. Catal. A: Gen. 582 (2019) 117108. doi: 10.1016/j.apcata.2019.06.006
16. [16]
  Y. Zuo, M. Liu, T. Zhang, et al., RSC Adv. 5 (2015) 17897–17904. doi: 10.1039/C5RA00194C
17. [17]
  Y.Y. Wang, L. Li, R.S. Bai, et al., Chin. J. Catal. 42 (2021) 2189–2196. doi: 10.1016/S1872-2067(21)63882-2
18. [18]
  Q. Guo, K.J. Sun, Z.C. Feng, et al., Chem. Eur. J. 18 (2012) 13854–13860. doi: 10.1002/chem.201201319
19. [19]
  W.J. Xu, T.J. Zhang, R.S. Bai, et al., J. Mater. Chem. A 8 (2020) 9677–9683. doi: 10.1039/C9TA13851J
20. [20]
  L.D. Sanchez, S. Taxt-Lamolle, E.O. Hole, et al., Appl. Catal. B: Environ. 142 (2013) 662–667.
21. [21]
  L.Z. Wu, X.J. Deng, S.F. Zhao, et al., Chem. Commun. 52 (2016) 8679–8682. doi: 10.1039/C6CC03318K
22. [22]
  J.P. Yin, H. Xu, B.W. Wang, et al., Catal. Sci. Technol. 10 (2020) 6050–6064. doi: 10.1039/D0CY00478B
23. [23]
  L. Xu, D.D. Huang, C.G. Li, et al., Chem. Commun. 51 (2015) 9010–9013. doi: 10.1039/C5CC02321A
24. [24]
  W.J. Zhou, R. Wischert, K. Xue, et al., ACS Catal. 4 (2014) 53–62. doi: 10.1021/cs400757j
25. [25]
  M. Dan-Hardi, C. Serre, T. Frot, et al., J. Am. Chem. Soc. 131 (2009) 10857. doi: 10.1021/ja903726m
26. [26]
  H. Wang, X.Z. Yuan, Y. Wu, et al., J. Hazard. Mater. 286 (2015) 187–194. doi: 10.1016/j.jhazmat.2014.11.039
27. [27]
  I.D. Ivanchikova, J.S. Lee, N.V. Maksimchuk, et al., Eur. J. Inorg. Chem. 2014 (2014) 132–139. doi: 10.1002/ejic.201301098
28. [28]
  N. Maksimchuk, J.S. Lee, A. Ayupov, et al., Catalysts 9 (2019) 324. doi: 10.3390/catal9040324
29. [29]
  X.M. Cheng, X.Y. Dao, S.Q. Wang, et al., ACS Catal. 11 (2021) 650–658. doi: 10.1021/acscatal.0c04426
30. [30]
  P. Yang, Y. Huang, Z.W. Zhang, et al., Dalton Trans. 49 (2020) 10052–10057. doi: 10.1039/D0DT01955K
31. [31]
  T.L. Lu, J.P. Zou, Y.Z. Zhan, et al., ACS Catal. 8 (2018) 1287–1296. doi: 10.1021/acscatal.7b03558
32. [32]
  F. Bonino, A. Damin, G. Ricchiardi, et al., J. Phys. Chem. B 108 (2004) 3573–3583. doi: 10.1021/jp036166e
33. [33]
  Z.Q. Yang, J. Ding, J.N. Feng, et al., Appl. Organomet. Chem. 32 (2018) e4285. doi: 10.1002/aoc.4285
34. [34]
  Z.M. Liu, Y.C. Wu, J.T. Chen, et al., Catal. Sci. Technol. 8 (2018) 1936–1944. doi: 10.1039/C8CY00125A
35. [35]
  O.A. Kholdeeva, T.A. Trubitsina, G.M. Maksimov, et al., Inorg. Chem. 44 (2005) 1635–1642. doi: 10.1021/ic0490829
36. [36]
  S. Bordiga, A. Damin, F. Bonino, et al., Angew. Chem. Int. Ed. 41 (2002) 4734–4737. doi: 10.1002/anie.200290032
37. [37]
  H.X. Guo, D. Guo, Z.S. Zheng, et al., Appl. Organomet. Chem. 29 (2015) 618–623. doi: 10.1002/aoc.3341
38. [38]
  H.H. Kim, H. Lee, D. Lee, et al., Environ. Sci. Technol. 54 (2020) 15424–15432. doi: 10.1021/acs.est.0c04262
39. [39]
  Z.J. Wu, K. Guo, S. Cao, et al., Nano Res. 13 (2020) 551–556. doi: 10.1007/s12274-020-2650-y
40. [40]
  D.H. Kim, A.D. Bokare, M.S. Koo, et al., Environ. Sci. Technol. 49 (2015) 3506–3513. doi: 10.1021/es5056897
41. [41]
  N. Chen, G.D. Fang, C.Y. Zhu, et al., J. Hazard. Mater. 389 (2020) 121819. doi: 10.1016/j.jhazmat.2019.121819
42. [42]
  G.D. Fang, Y.M. Deng, M. Huang, et al., Environ. Sci. Technol. 52 (2018) 2178–2185. doi: 10.1021/acs.est.7b05303
43. [43]
  Y. Liu, H. Guo, Y. Zhang, et al., Chem. Eng. J. 343 (2018) 10.
44. [44]
  C.W. Yoon, K.F. Hirsekorn, M.L. Neidig, et al., ACS Catal. 1 (2011) 1665–1678. doi: 10.1021/cs2003774
45. [45]
  Y. Zhou, S. Feng, X.M. Duan, et al., J. Solid State Chem. 300 (2021) 122231. doi: 10.1016/j.jssc.2021.122231
46. [46]
  G. Pan, J. Wei, M. Xu, et al., J. Hazard. Mater. 445 (2022) 130479.
47. [47]
  C.P. Gordon, H. Engler, A.S. Tragl, et al., Nature 586 (2020) 708–713. doi: 10.1038/s41586-020-2826-3
1. [1]
  Ruonan Guo , Heng Zhang , Changsheng Guo , Ningqing Lv , Beidou Xi , Jian Xu . Degradation of neonicotinoids with different molecular structures in heterogeneous peroxymonosulfate activation system through different oxidation pathways. Chinese Chemical Letters, 2024, 35(9): 109413-. doi: 10.1016/j.cclet.2023.109413
2. [2]
  Tengjia Ni , Xianbiao Hou , Huanlei Wang , Lei Chu , Shuixing Dai , Minghua Huang . Controllable defect engineering based on cobalt metal-organic framework for boosting oxygen evolution reaction. Chinese Journal of Structural Chemistry, 2024, 43(1): 100210-100210. doi: 10.1016/j.cjsc.2023.100210
3. [3]
  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
4. [4]
  Jiayu Huang , Kuan Chang , Qi Liu , Yameng Xie , Zhijia Song , Zhiping Zheng , Qin Kuang . Fe-N-C nanostick derived from 1D Fe-ZIFs for Electrocatalytic oxygen reduction. Chinese Journal of Structural Chemistry, 2023, 42(10): 100097-100097. doi: 10.1016/j.cjsc.2023.100097
5. [5]
  Longlong Geng , Huiling Liu , Wenfeng Zhou , Yong-Zheng Zhang , Hongliang Huang , Da-Shuai Zhang , Hui Hu , Chao Lv , Xiuling Zhang , Suijun Liu . Construction of metal-organic frameworks with unsaturated Cu sites for efficient and fast reduction of nitroaromatics: A combined experimental and theoretical study. Chinese Chemical Letters, 2024, 35(8): 109120-. doi: 10.1016/j.cclet.2023.109120
6. [6]
  Rui Wang , He Qi , Haijiao Zheng , Qiong Jia . Light/pH dual-responsive magnetic metal-organic frameworks composites for phosphorylated peptide enrichment. Chinese Chemical Letters, 2024, 35(7): 109215-. doi: 10.1016/j.cclet.2023.109215
7. [7]
  Xiao-Hong Yi , Chong-Chen Wang . Metal-organic frameworks on 3D interconnected macroporous sponge foams for large-scale water decontamination: A mini review. Chinese Chemical Letters, 2024, 35(5): 109094-. doi: 10.1016/j.cclet.2023.109094
8. [8]
  Yuan Zhang , Shenghao Gong , A.R. Mahammed Shaheer , Rong Cao , Tianfu Liu . Plasmon-enhanced photocatalytic oxidative coupling of amines in the air using a delicate Ag nanowire@NH₂-UiO-66 core-shell nanostructures. Chinese Chemical Letters, 2024, 35(4): 108587-. doi: 10.1016/j.cclet.2023.108587
9. [9]
  Zhi Wang , Lingpeng Yan , Yelin Hao , Jingxia Zheng , Yongzhen Yang , Xuguang Liu . Highly efficient and photothermally stable CDs@ZIF-8 for laser illumination. Chinese Chemical Letters, 2024, 35(10): 109430-. doi: 10.1016/j.cclet.2023.109430
10. [10]
  Hao Wang , Meng-Qi Pan , Ya-Fei Wang , Chao Chen , Jian Xu , Yuan-Yuan Gao , Chuan-Song Qi , Wei Li , Xian-He Bu . Post-synthetic modifications of MOFs by different bolt ligands for controllable release of cargoes. Chinese Chemical Letters, 2024, 35(10): 109581-. doi: 10.1016/j.cclet.2024.109581
11. [11]
  Zhiqiang Liu , Qiang Gao , Wei Shen , Meifeng Xu , Yunxin Li , Weilin Hou , Hai-Wei Shi , Yaozuo Yuan , Erwin Adams , Hian Kee Lee , Sheng Tang . Removal and fluorescence detection of antibiotics from wastewater by layered double oxides/metal-organic frameworks with different topological configurations. Chinese Chemical Letters, 2024, 35(8): 109338-. doi: 10.1016/j.cclet.2023.109338
12. [12]
  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
13. [13]
  Xueyang Zhao , Bangwei Deng , Hongtao Xie , Yizhao Li , Qingqing Ye , Fan Dong . Recent process in developing advanced heterogeneous diatomic-site metal catalysts for electrochemical CO₂ reduction. Chinese Chemical Letters, 2024, 35(7): 109139-. doi: 10.1016/j.cclet.2023.109139
14. [14]
  Weixu Li , Yuexin Wang , Lin Li , Xinyi Huang , Mengdi Liu , Bo Gui , Xianjun Lang , Cheng Wang . Promoting energy transfer pathway in porphyrin-based sp2 carbon-conjugated covalent organic frameworks for selective photocatalytic oxidation of sulfide. Chinese Journal of Structural Chemistry, 2024, 43(7): 100299-100299. doi: 10.1016/j.cjsc.2024.100299
15. [15]
  Xiaoyan Peng , Xuanhao Wu , Fan Yang , Yefei Tian , Mingming Zhang , Hongye Yuan . Gas sensors based on metal-organic frameworks: challenges and opportunities. Chinese Journal of Structural Chemistry, 2024, 43(3): 100251-100251. doi: 10.1016/j.cjsc.2024.100251
16. [16]
  Kang Wang , Qinglin Zhou , Weijin Li . Conductive metal-organic frameworks for electromagnetic wave absorption. Chinese Journal of Structural Chemistry, 2024, 43(10): 100325-100325. doi: 10.1016/j.cjsc.2024.100325
17. [17]
  Ruikui YAN , Xiaoli CHEN , Miao CAI , Jing REN , Huali CUI , Hua YANG , Jijiang WANG . Design, synthesis, and fluorescence sensing performance of highly sensitive and multi-response lanthanide metal-organic frameworks. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 834-848. doi: 10.11862/CJIC.20230301
18. [18]
  Jian Yang , Guang Yang , Zhijie Chen . Capturing carbon dioxide from air by using amine-functionalized metal-organic frameworks. Chinese Journal of Structural Chemistry, 2024, 43(5): 100267-100267. doi: 10.1016/j.cjsc.2024.100267
19. [19]
  Xian-Fa Jiang , Chongyun Shao , Zhongwen Ouyang , Zhao-Bo Hu , Zhenxing Wang , You Song . Generating electron spin qubit in metal-organic frameworks via spontaneous hydrolysis. Chinese Chemical Letters, 2024, 35(7): 109011-. doi: 10.1016/j.cclet.2023.109011
20. [20]
  Xue-Zhi Wang , Yi-Tong Liu , Chuang-Wei Zhou , Bei Wang , Dong Luo , Mo Xie , Meng-Ying Sun , Yong-Liang Huang , Jie Luo , Yan Wu , Shuixing Zhang , Xiao-Ping Zhou , Dan Li . Amplified circularly polarized luminescence of chiral metal-organic frameworks via post-synthetic installing pillars. Chinese Chemical Letters, 2024, 35(10): 109380-. doi: 10.1016/j.cclet.2023.109380

Get Citation

PDF

XML

Metrics

PDF Downloads(1)
Abstract views(93)
HTML views(1)

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