Citation: Qian Liu, Hui Li, Hao Zhang, Zhurui Shen, Huiming Ji. The role of Cs dopants for improved activation of molecular oxygen and degradation of tetracycline over carbon nitride[J]. Chinese Chemical Letters, ;2022, 33(11): 4756-4760. doi: 10.1016/j.cclet.2021.12.089 shu

The role of Cs dopants for improved activation of molecular oxygen and degradation of tetracycline over carbon nitride

Qian Liu ^a ,
Hui Li ^b ,
Hao Zhang ^b ,
Zhurui Shen ^{b, *,} ,
Huiming Ji ^a

a.
School of Materials Science and Engineering, Key Laboratory of Advanced Ceramics and Machining Technology, Ministry of Education, Tianjin University, Tianjin 300350, China
b.
School of Materials Science and Engineering, Nankai University, Tianjin 300350, China

shenzhurui@nankai.edu.cn

Received Date: 27 September 2021
Revised Date: 29 October 2021
Accepted Date: 31 December 2021
Available Online: 7 January 2022

Figures(6)

Molecular oxygen (O₂) is activated to reactive oxygen species (ROS) by transferring energy and carriers in the photocatalytic process, which plays an important role in environmental remediation. Herein, Cs-doped carbon nitride (CN-xCs, x = 0.2, 0.8, 1) was prepared by CsCl directly inducing the structural reconstruction of carbon nitride (CN), which had obvious molecular oxygen activation ability to promote tetracycline (TC) degradation. Besides, we explored the influence of Cs doping concentration. As a consequence, the doping concentration of Cs was an important factor affecting the activation of O₂, which could cause changes in the physical and chemical structure of CN, make O enter the CN structure, form N vacancy defects and cyano groups. In addition, a proper amount of Cs doping could reduce the band gap value, increase the light absorption range, have better charge separation and transfer performance, which could remarkably promote the activation of O₂. Benefiting from these advantages, CN-0.8Cs could generate a higher concentration of superoxide radicals (^•O₂⁻, 179.30 µmol/L), which was much higher than CN (6.22 µmol/L). Therefore, it exhibited excellent TC degradation photocatalytic performance, and the rate constant k of TC degradation was 0.020 min⁻¹, which was 6.7 times the degradation rate of CN (k = 0.0030 min⁻¹). Furthermore, the possible degradation pathways of TC were proposed based on the results of HPLC-MS.
- O₂ activation,
- Reactive oxygen species,
- Cs doping of CN,
- Degradation and mineralization,
- Tetracycline
1. [1]
  M. Zhang, C. Lai, B. Li, et al., Chem. Eng. J. 396 (2020) 125343. doi: 10.1016/j.cej.2020.125343
2. [2]
  Q. Li, F. Li, Chem. Eng. J. 421 (2021) 129915. doi: 10.1016/j.cej.2021.129915
3. [3]
  H. Li, S. Sun, H. Ji, et al., Appl. Catal. B 272 (2020) 118966. doi: 10.1016/j.apcatb.2020.118966
4. [4]
  Z. Zhou, Z. Shen, C. Song, et al., Water Res. 201 (2021) 117314. doi: 10.1016/j.watres.2021.117314
5. [5]
  J. Xiao, Q. Han, Y. Xie, et al., Environ. Sci. Technol. 51 (2017) 13380–13387. doi: 10.1021/acs.est.7b04215
6. [6]
  Y. Cao, Q. Zheng, Z. Rao, et al., Chin. Chem. Lett. 31 (2020) 2689–2692. doi: 10.1016/j.cclet.2020.07.032
7. [7]
  N. Tian, H. Huang, X. Du, F. Dong, Y. Zhang, J. Mater. Chem. A 7 (2019) 11584–11612. doi: 10.1039/C9TA01819K
8. [8]
  C. Wang, M. Fu, J. Cao, et al., Chem. Eng. J. 385 (2020) 123833. doi: 10.1016/j.cej.2019.123833
9. [9]
  H. Wang, J. Zhang, P. Wang, et al., Chin. Chem. Lett. 31 (2020) 2789–2794. doi: 10.1016/j.cclet.2020.07.043
10. [10]
  B. Zhang, C. Li, Y. Zhang, et al., Sci. Total Environ. 757 (2021) 143810. doi: 10.1016/j.scitotenv.2020.143810
11. [11]
  D. Zhang, X. Han, T. Dong, et al., J. Catal. 366 (2018) 237–244. doi: 10.1016/j.jcat.2018.08.018
12. [12]
  X. Hu, P. Lu, Y. He, et al., Appl. Surf. Sci. 528 (2020) 146924. doi: 10.1016/j.apsusc.2020.146924
13. [13]
  X. Hu, P. Lu, R. Pan, et al., Chem. Eng. J. 423 (2021) 130278. doi: 10.1016/j.cej.2021.130278
14. [14]
  X. Liu, W. Yu, C. Li, et al., J. Agric. Food Chem. 69 (2021) 28–35. doi: 10.1021/acs.jafc.0c03648
15. [15]
  X. Li, S. Lyu, X. Lang, Environ. Res. 195 (2021) 110851. doi: 10.1016/j.envres.2021.110851
16. [16]
  M. Zhang, C. Lai, B. Li, et al., Chem. Eng. J. 422 (2021) 130120. doi: 10.1016/j.cej.2021.130120
17. [17]
  J. Dai, J. Song, Y. Qiu, et al., ACS Appl. Mater. Interfaces 11 (2019) 10589–10596. doi: 10.1021/acsami.9b01307
18. [18]
  X. Liu, C. Li, Y. Zhang, et al., Appl. Catal. B 219 (2017) 194–199. doi: 10.1016/j.apcatb.2017.07.007
19. [19]
  L. Lin, H. Ou, Y. Zhang, et al., ACS Catal. 6 (2016) 3921–3931. doi: 10.1021/acscatal.6b00922
20. [20]
  W. Yan, L. Yan, C. Jing, Appl. Catal. B 244 (2019) 475–485. doi: 10.1016/j.apcatb.2018.11.069
21. [21]
  L. Lin, Z. Yu, X. Wang, Angew. Chem. Int. Ed. 131 (2019) 6225–6236. doi: 10.1002/ange.201809897
22. [22]
  S. Wu, H. Yu, S. Chen, et al., ACS Catal. 10 (2020) 14380–14389. doi: 10.1021/acscatal.0c03359
23. [23]
  Y. Xu, Y. Gong, H. Ren, et al., RSC Adv. 7 (2017) 32592–32600. doi: 10.1039/C7RA05555B
24. [24]
  K. Mori, D. Tatsumi, T. Iwamoto, et al., Chem. Eur. J. 13 (2018) 1348–1356.
25. [25]
  K. Bai, Z. Cui, E. Li, et al., Mod. Phys. Lett. B 34 (2020) 2050361. doi: 10.1142/S0217984920503613
26. [26]
  H. Zhang, Y. Tang, Z. Liu, et al., Chem. Phys. Lett. 751 (2020) 137467. doi: 10.1016/j.cplett.2020.137467
27. [27]
  B.V. Lotsch, M. Döblinger, J. Sehnert, et al., Chem. Eur. J. 13 (2007) 4969–4980. doi: 10.1002/chem.200601759
28. [28]
  S. Cao, J. Low, J. Yu, et al., Adv. Mater. 27 (2015) 2150–2176. doi: 10.1002/adma.201500033
29. [29]
  P. Niu, L. Zhang, G. Liu, H. Cheng, Adv. Funct. Mater. 22 (2012) 4763–4770. doi: 10.1002/adfm.201200922
30. [30]
  T. Xiong, W. Cen, Y. Zhang, F. Dong, ACS Catal. 6 (2016) 2462–2472. doi: 10.1021/acscatal.5b02922
31. [31]
  G. Zhang, G. Li, Z. Lan, et al., Angew. Chem. Int. Ed. 56 (2017) 13445–13449. doi: 10.1002/anie.201706870
32. [32]
  H. Lan, L. Li, X. An, et al., Appl. Catal. B 204 (2017) 49–57. doi: 10.1016/j.apcatb.2016.11.022
33. [33]
  C. Chang, Y. Fu, M. Hu, et al., Appl. Catal. B 142 (2013) 553–560.
34. [34]
  X.L. Wang, W.Q. Fang, N. Abbas, et al., J. Mater. Chem. A 1 (2013) 14089–14096. doi: 10.1039/c3ta13328a
35. [35]
  V.W. Lau, V.W. Yu, F. Ehrat, et al., Adv. Energy Mater. 7 (2017) 1602251. doi: 10.1002/aenm.201602251
36. [36]
  H. Yu, R. Shi, Y. Zhao, et al., Adv. Mater. 29 (2017) 1605148. doi: 10.1002/adma.201605148
37. [37]
  L. Luo, T. Zhang, M. Wang, et al., ChemSusChem 13 (2020) 5173–5184. doi: 10.1002/cssc.202001398
38. [38]
  W. Zhang, L. Zhou, J. Shi, et al., J. Colloid Interface Sci. 496 (2017) 167–176. doi: 10.1016/j.jcis.2017.02.022
39. [39]
  P. Qiu, C. Xu, H. Chen, et al., Appl. Catal. B 206 (2017) 319–327. doi: 10.1016/j.apcatb.2017.01.058
40. [40]
  P. Chen, L. Blaney, G. Cagnetta, et al., Environ. Sci. Technol. 53 (2019) 1564–1575. doi: 10.1021/acs.est.8b05827
41. [41]
  S. Jiao, S. Zheng, D. Yin, L. Wang, L. Chen, Chemosphere 73 (2008) 377–382. doi: 10.1016/j.chemosphere.2008.05.042
42. [42]
  B. Balci, N. Oturan, R. Cherrier, et al., Water Res. 43 (2009) 1924–1934. doi: 10.1016/j.watres.2009.01.021
43. [43]
  V.M. Mboula, V. Hequet, Y. Gru, et al., J. Hazard. Mater. 209 (2012) 355–364.
1. [1]
  Kai Han , Guohui Dong , Ishaaq Saeed , Tingting Dong , Chenyang Xiao . Morphology and photocatalytic tetracycline degradation of g-C3N4 optimized by the coal gangue. Chinese Journal of Structural Chemistry, 2024, 43(2): 100208-100208. doi: 10.1016/j.cjsc.2023.100208
2. [2]
  Fengrui Yang , Debing Wang , Xinying Zhang , Jie Zhang , Zhichao Wu , Qiaoying Wang . Synergistic effects of peroxydisulfate on UV/O₃ process for tetracycline degradation: Mechanism and pathways. Chinese Chemical Letters, 2024, 35(10): 109599-. doi: 10.1016/j.cclet.2024.109599
3. [3]
  Ruru Li , Qian Liu , Hui Li , Fengbin Sun , Zhurui Shen . Rational design of dual sites induced local electron rearrangement for enhanced photocatalytic oxygen activation. Chinese Chemical Letters, 2024, 35(11): 109679-. doi: 10.1016/j.cclet.2024.109679
4. [4]
  Xin Li , Wanting Fu , Ruiqing Guan , Yue Yuan , Qinmei Zhong , Gang Yao , Sheng-Tao Yang , Liandong Jing , Song Bai . Nucleophiles promotes the decomposition of electrophilic functional groups of tetracycline in ZVI/H₂O₂ system: Efficiency and mechanism. Chinese Chemical Letters, 2024, 35(10): 109625-. doi: 10.1016/j.cclet.2024.109625
5. [5]
  Zhongyu Wang , Lijun Wang , Huaixin Zhao . DNA-based nanosystems to generate reactive oxygen species for nanomedicine. Chinese Chemical Letters, 2024, 35(11): 109637-. doi: 10.1016/j.cclet.2024.109637
6. [6]
  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
7. [7]
  Kun-Heng Li , Hong-Yang Zhao , Dan-Dan Wang , Ming-Hui Qi , Zi-Jian Xu , Jia-Mi Li , Zhi-Li Zhang , Shi-Wen Huang . Mitochondria-targeted nano-AIEgens as a powerful inducer for evoking immunogenic cell death. Chinese Chemical Letters, 2024, 35(5): 108882-. doi: 10.1016/j.cclet.2023.108882
8. [8]
  Feifei Wang , Hang Yao , Xinyue Wu , Yijian Tang , Yang Bai , Hui Chong , Huan Pang . Metal–organic framework and its composites modulate macrophage polarization in the treatment of inflammatory diseases. Chinese Chemical Letters, 2024, 35(5): 108821-. doi: 10.1016/j.cclet.2023.108821
9. [9]
  Yihao Zhang , Yang Jiao , Xianchao Jia , Qiaojia Guo , Chunying Duan . Highly effective self-assembled porphyrin MOCs nanomaterials for enhanced photodynamic therapy in tumor. Chinese Chemical Letters, 2024, 35(5): 108748-. doi: 10.1016/j.cclet.2023.108748
10. [10]
  Jiaqi Huang , Renjiang Kong , Yanmei Li , Ni Yan , Yeyang Wu , Ziwen Qiu , Zhenming Lu , Xiaona Rao , Shiying Li , Hong Cheng . Feedback enhanced tumor targeting delivery of albumin-based nanomedicine to amplify photodynamic therapy by regulating AMPK signaling and inhibiting GSTs. Chinese Chemical Letters, 2024, 35(8): 109254-. doi: 10.1016/j.cclet.2023.109254
11. [11]
  Haijing Cui , Weihao Zhu , Chuning Yue , Ming Yang , Wenzhi Ren , Aiguo Wu . Recent progress of ultrasound-responsive titanium dioxide sonosensitizers in cancer treatment. Chinese Chemical Letters, 2024, 35(10): 109727-. doi: 10.1016/j.cclet.2024.109727
12. [12]
  Qinyu Zhao , Yunchao Zhao , Songjing Zhong , Zhaoyang Yue , Zhuoheng Jiang , Shaobo Wang , Quanhong Hu , Shuncheng Yao , Kaikai Wen , Linlin Li . Urchin-like piezoelectric ZnSnO₃/Cu₃P p-n heterojunction for enhanced cancer sonodynamic therapy. Chinese Chemical Letters, 2024, 35(12): 109644-. doi: 10.1016/j.cclet.2024.109644
13. [13]
  Xiangdong Lai , Tengfei Liu , Zengchao Guo , Yihan Wang , Jiang Xiao , Qingxiu Xia , Xiaohui Liu , Hui Jiang , Xuemei Wang . In situ formed fluorescent gold nanoclusters inhibit hair follicle regeneration in oxidative stress microenvironment via suppressing NFκB signal pathway. Chinese Chemical Letters, 2025, 36(2): 109762-. doi: 10.1016/j.cclet.2024.109762
14. [14]
  Zekun Gao , Xiuli Zheng , Weimin Liu , Jie Sha , Shuaishuai Bian , Haohui Ren , Jiasheng Wu , Wenjun Zhang , Chun-Sing Lee , Pengfei Wang . GSH-activatable copper-elsinochrome off-on photosensitizer for combined specific NIR-Ⅱ two-photon photodynamic/chemodynamic therapy. Chinese Chemical Letters, 2025, 36(3): 109874-. doi: 10.1016/j.cclet.2024.109874
15. [15]
  Chi Zhang , Ning Ding , Yuwei Pan , Lichun Fu , Ying Zhang . The degradation pathways of contaminants by reactive oxygen species generated in the Fenton/Fenton-like systems. Chinese Chemical Letters, 2024, 35(10): 109579-. doi: 10.1016/j.cclet.2024.109579
16. [16]
  Zhinan GUO , Junli WANG , Qiang ZHAO , Zhifang JIA , Zuopeng LI , Kewei WANG , Yong GUO . Cu₂O/Bi₂CrO₆ Z-scheme heterojunction: Construction and photocatalytic degradation properties for tetracycline. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 741-752. doi: 10.11862/CJIC.20240403
17. [17]
  Renshu Huang , Jinli Chen , Xingfa Chen , Tianqi Yu , Huyi Yu , Kaien Li , Bin Li , Shibin Yin . Synergized oxygen vacancies with Mn2O3@CeO2 heterojunction as high current density catalysts for Li–O2 batteries. Chinese Journal of Structural Chemistry, 2023, 42(11): 100171-100171. doi: 10.1016/j.cjsc.2023.100171
18. [18]
  Yuanyi Zhou , Ke Ma , Jinfeng Liu , Zirun Zheng , Bo Hu , Yu Meng , Zhizhong Li , Mingshan Zhu . Is reactive oxygen species the only way for cancer inhibition over single atom nanomedicine? Autophagy regulation also works. Chinese Chemical Letters, 2024, 35(6): 109056-. doi: 10.1016/j.cclet.2023.109056
19. [19]
  Ruiheng Liang , Huizhong Wu , Zhongzheng Hu , Ge Song , Xuyang Zhang , Omotayo A. Arotiba , Minghua Zhou . Hierarchical Fe-Bi/Bi₇O₉I₃/OVs microspheres coupled with natural air diffusion electrode to achieve efficient heterogeneous visible-light-driven photoelectro-Fenton degradation of tetracycline without aeration. Chinese Chemical Letters, 2025, 36(4): 110136-. doi: 10.1016/j.cclet.2024.110136
20. [20]
  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. Chinese Chemical Letters, 2024, 35(5): 108903-. doi: 10.1016/j.cclet.2023.108903

Get Citation

PDF

XML

Metrics

PDF Downloads(8)
Abstract views(781)
HTML views(67)

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