Citation: Denghong Zhao, Mingwei Yang, Yichuan Zhang, Long Qin, Hang Liu, Hongji Chen, Maoguo Tan, Zhongyi Yin, Bin Sun, Yu Shen, Haijiao Xie, Heyan Jiang. Microwave assisted metal-free catalysts preparation from waste plastics for efficient pollutants degradation: Interesting relationship between plastic types and nonradical/radical pathways[J]. Chinese Chemical Letters, ;2026, 37(3): 111631. doi: 10.1016/j.cclet.2025.111631 shu

Microwave assisted metal-free catalysts preparation from waste plastics for efficient pollutants degradation: Interesting relationship between plastic types and nonradical/radical pathways

Denghong Zhao ^a ,
Mingwei Yang ^a ,
Yichuan Zhang ^a ,
Long Qin ^a ,
Hang Liu ^a ,
Hongji Chen ^a ,
Maoguo Tan ^a ,
Zhongyi Yin ^a ,
Bin Sun ^a ,
Yu Shen ^a ,
Haijiao Xie ^b ,
Heyan Jiang ^{a, *,}

a.
Key Laboratory of Catalysis Science and Technology of Chongqing Education Commission, Chongqing Key Laboratory of Environmental Catalysis, Chongqing Technology and Business University, Chongqing 400067, China
b.
Hangzhou Yanqu Information Technology Co., Ltd., Hangzhou 310003, China

orgjiang@163.com

Received Date: 22 February 2025
Revised Date: 6 June 2025
Accepted Date: 22 July 2025
Available Online: 25 July 2025

Figures(6)

To implement the principle of utilizing waste to address waste issues, porous carbon catalytic materials, prepared through a straightforward process involving NaOH-assisted microwave pyrolysis of ubiquitous waste plastics, were employed to degrade pollutants via peroxymonosulfate (PMS) activation. Polyethylene terephthalate (PET) derived P₁S₂ exhibited characteristics of defects enrichment and CO formation, while H₁S₂, prepared by carbonization of high-density polyethylene (HDPE), possessed a large number of COH and defects. Metal-free catalysts P₁S₂ and H₁S₂ exhibited excellent tetracycline (TC) degradation performance, with the rate constants up to 0.303 min^-1 and 0.235 min^-1. Interestingly, mechanism studies demonstrated that the types of waste plastic precursor had a significant impact on the pathways involved in TC degradation. Specifically, carbon defects in P₁S₂ dominated the electron transfer nonradial degradation pathway of TC; However, COH in H₁S₂ served as the reactive site for main active species SO₄^•−/^•OH generation, initiating a free radical pathway. In addition, by combining Fukui function calculation and LC-MS test during the TC degradation process, the vulnerable sites attacked by active species were identified; different degradation routes of TC in nonradial and radial pathways were proposed and discussed. Furthermore, the toxicity of all intermediates was analyzed using the toxicity assessment software. This study offers fresh insights into the critical role of carbocatalysts derived from various waste plastics in both nonradical and radical activation processes of PMS.
- Waste plastic,
- Porous carbon material,
- Microwave pyrolysis,
- Peroxymonosulfate,
- Nonradical/radical pathways
1. [1]
  W. Wang, X. Li, F. Deng, et al., Chin. Chem. Lett. 33 (2022) 5200–5207. doi: 10.1016/j.cclet.2022.01.058
2. [2]
  Y. Hu, F.L. Meng, J.H. Zhao, et al., Water Res. 262 (2024) 122112. doi: 10.1016/j.watres.2024.122112
3. [3]
  Y. Li, M. Fan, C. Wang, et al., Chin. Chem. Lett. 35 (2024) 109764. doi: 10.1016/j.cclet.2024.109764
4. [4]
  X. Mao, M. Wang, J. Li, et al., Appl. Catal. B: Environ. 331 (2023) 122698. doi: 10.1016/j.apcatb.2023.122698
5. [5]
  L. Hu, Y. Zhang, X. Liu, et al., Chem. Eng. J. 450 (2022) 138219. doi: 10.1016/j.cej.2022.138219
6. [6]
  R. Ji, J. Chen, T. Liu, X. Zhou, Y. Zhang, Chin. Chem. Lett. 33 (2022) 643–652. doi: 10.1016/j.cclet.2021.07.043
7. [7]
  J. Xu, J. Song, Y. Min, Q. Xu, P. Shi, Chin. Chem. Lett. 33 (2022) 3113–3118. doi: 10.1016/j.cclet.2021.10.005
8. [8]
  J. Xie, L. Zhang, X. Luo, et al., Chem. Eng. J. 457 (2023) 141149. doi: 10.1016/j.cej.2022.141149
9. [9]
  H. Zhang, X. Gan, S. Chen, H. Yu, X. Quan, Sep. Purif. Technol. 292 (2022) 121048. doi: 10.1016/j.seppur.2022.121048
10. [10]
  M. Kohantorabi, G. Moussavi, S. Giannakis, et al., Chem. Eng. J. 411 (2021) 127957. doi: 10.1016/j.cej.2020.127957
11. [11]
  X. Duan, Z. Ao, L. Zhou, et al., Appl. Catal. B: Environ. 188 (2016) 98–105. doi: 10.1016/j.apcatb.2016.01.059
12. [12]
  J. Wang, X. Duan, J. Gao, et al., Water Res. 185 (2020) 116244. doi: 10.1016/j.watres.2020.116244
13. [13]
  J. Kang, X. Duan, L. Zhou, et al., Chem. Eng. J. 288 (2016) 399–405. doi: 10.1016/j.cej.2015.12.040
14. [14]
  J. Dou, J. Cheng, Z. Lu, et al., Appl. Catal. B: Environ. 301 (2022) 120832. doi: 10.1016/j.apcatb.2021.120832
15. [15]
  F. Ye, Y. Su, R. Li, et al., Appl. Catal. B: Environ. 337 (2023) 122992. doi: 10.1016/j.apcatb.2023.122992
16. [16]
  X. Duan, H. Sun, Y. Wang, J. Kang, S. Wang, ACS Catal. 5 (2015) 553–559. doi: 10.1021/cs5017613
17. [17]
  P. Wang, H. Zhang, Z. Wu, et al., Chin. Chem. Lett. 34 (2023) 108722. doi: 10.1016/j.cclet.2023.108722
18. [18]
  J. Mehta, N. Dilbaghi, A. Deep, et al., Carbon 234 (2024) 119969.
19. [19]
  A. Stubbins, K.L. Law, S.E. Muñoz, T.S. Bianchi, L. Zhu, Science 373 (2021) 51–55. doi: 10.1126/science.abb0354
20. [20]
  Y. Luo, X. Lin, E. Lichtfouse, H. Jiang, C. Wang, Environ. Chem. Lett. 21 (2023) 3127–3158. doi: 10.1007/s10311-023-01638-7
21. [21]
  W.A. Algozeeb, P.E. Savas, Z. Yuan, et al., ACS Nano 16 (2022) 7284–7290. doi: 10.1021/acsnano.2c00955
22. [22]
  X. Duan, H. Sun, S. Wang, Acc. Chem. Res. 51 (2018) 678–687. doi: 10.1021/acs.accounts.7b00535
23. [23]
  S. Ren, X. Xu, Z.S. Zhu, et al., Appl. Catal. B: Environ. 342 (2024) 123410. doi: 10.1016/j.apcatb.2023.123410
24. [24]
  Q. Cao, X.F. Cheng, J. Wang, et al., Chin. Chem. Lett. 35 (2024) 108759. doi: 10.1016/j.cclet.2023.108759
25. [25]
  Q. Zhou, L. Qin, Z. Yin, H. Jiang, Sep. Purif. Technol. 328 (2024) 125033. doi: 10.1016/j.seppur.2023.125033
26. [26]
  H. Jiang, J. Zhou, Q. Zhou, et al., Chem. Eng. J. 489 (2024) 151256. doi: 10.1016/j.cej.2024.151256
27. [27]
  C. Gan, Q. Zhou, M. Sheng, et al., J. Clean. Prod. 434 (2024) 140417. doi: 10.1016/j.jclepro.2023.140417
28. [28]
  M. Sheng, C. Gan, Y. Li, et al., Appl. Catal. B: Environ. 339 (2023) 123138. doi: 10.1016/j.apcatb.2023.123138
29. [29]
  N. Cai, X. Li, S. Xia, et al., Energy Convers. Manage. 229 (2021) 113794. doi: 10.1016/j.enconman.2020.113794
30. [30]
  T. Kan, V. Strezov, T.J. Evans, Renew. Sust. Energy Rev. 57 (2016) 1126–1140. doi: 10.1016/j.rser.2015.12.185
31. [31]
  H. Zhang, T. Tao, X. Li, et al., Int. J. Hydrogen Energy 45 (2020) 18057–18065. doi: 10.1016/j.ijhydene.2020.04.190
32. [32]
  H. Yang, R. Qiu, Y. Tang, et al., Water Res. 231 (2023) 119659. doi: 10.1016/j.watres.2023.119659
33. [33]
  X. Li, T. Han, Y. Zhou, et al., Appl. Catal. B: Environ. 350 (2024) 123913. doi: 10.1016/j.apcatb.2024.123913
34. [34]
  S. Zhao, S.S. Shen, L. Han, B.C. Tian, N. Li, W. Chen, X.B. Li, Rare Met. 43 (2024) 4038–4055. doi: 10.1007/s12598-024-02847-x
35. [35]
  Q. Zhou, L. Qin, H. Liu, et al., Chem. Eng. J. 487 (2024) 150370. doi: 10.1016/j.cej.2024.150370
36. [36]
  C. Gan, M. Sheng, Z. Hu, et al., J. Catal. 413 (2022) 636–647. doi: 10.1016/j.jcat.2022.07.022
37. [37]
  J.C.E. Yang, M.P. Zhu, D.D. Dionysiou, et al., Chem. Eng. J. 430 (2022) 133102. doi: 10.1016/j.cej.2021.133102
38. [38]
  J. Wu, J. Wang, C. Liu, et al., Environ. Sci. Technol. 56 (2022) 13996–14007. doi: 10.1021/acs.est.2c03590
39. [39]
  W. Tian, H. Zhang, X. Duan, et al., ACS Appl. Mater. Interfaces 8 (2016) 7184–7193. doi: 10.1021/acsami.6b01748
40. [40]
  H. Li, X. Zhang, S. Yang, Y. Sun, J. Qian, Environ. Sci. Technol. 58 (2024) 14005–14012. doi: 10.1021/acs.est.4c02809
41. [41]
  S. Ma, D. Yang, Y. Guan, et al., Appl. Catal. B: Environ. 316 (2022) 121594. doi: 10.1016/j.apcatb.2022.121594
42. [42]
  F. Li, Z. Lu, T. Li, P. Zhang, C. Hu, Environ. Sci. Technol. 56 (2022) 8765–8775. doi: 10.1021/acs.est.2c00369
43. [43]
  Y. Wang, Y. Song, N. Li, et al., J. Hazard. Mater. 421 (2022) 126794. doi: 10.1016/j.jhazmat.2021.126794
44. [44]
  Y. Qi, B. Ge, Y. Zhang, et al., J. Hazard. Mater. 399 (2020) 123039. doi: 10.1016/j.jhazmat.2020.123039
45. [45]
  B. Zhou, L. Chen, F. Li, et al., Chin. Chem. Lett. 34 (2023) 108558. doi: 10.1016/j.cclet.2023.108558
46. [46]
  M. Zhang, J. Ruan, X. Wang, et al., Water Res. 246 (2023) 120697. doi: 10.1016/j.watres.2023.120697
47. [47]
  Z. Xu, Y. Zhang, F. Wang, et al., Chem. Eng. J. 452 (2023) 139229. doi: 10.1016/j.cej.2022.139229
48. [48]
  F. Wang, S.S. Liu, Z. Feng, et al., J. Hazard. Mater. 440 (2022) 129723. doi: 10.1016/j.jhazmat.2022.129723
49. [49]
  X. Li, S. Wang, P. Chen, et al., Appl. Catal. B: Environ. 325 (2023) 122401. doi: 10.1016/j.apcatb.2023.122401
50. [50]
  F. Sun, X. Yang, F. Shao, et al., Chin. Chem. Lett. 34 (2023) 108563. doi: 10.1016/j.cclet.2023.108563
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2. [2]
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