Citation: Fei Ye, Yan Liu, Qianru Lv, Boru Gao, Jingjing Xia, Xinyu Li, Mengmeng Dou, Kun Zhao, Munir Ahmad, Zhourong Xiao, Sufeng Wang, Shuaijie Wang, Qingrui Zhang. Unveiling the mechanism of efficient detoxification by Pd species in chlorinated pollutant degradation[J]. Chinese Chemical Letters, ;2026, 37(2): 111136. doi: 10.1016/j.cclet.2025.111136 shu

Unveiling the mechanism of efficient detoxification by Pd species in chlorinated pollutant degradation

Fei Ye ^{a, 1} ,
Yan Liu ^{a, 1} ,
Qianru Lv ^a ,
Boru Gao ^{b, *,} ,
Jingjing Xia ^a ,
Xinyu Li ^c ,
Mengmeng Dou ^c ,
Kun Zhao ^d ,
Munir Ahmad ^e ,
Zhourong Xiao ^a ,
Sufeng Wang ^a ,
Shuaijie Wang ^a ,
Qingrui Zhang ^{a, *,}

a.
State Key Laboratory of Metastable Materials Science and Technology, Hebei Key Laboratory of Heavy Metal Deep-Remediation in Water and Resource Reuse, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao 066004, China
b.
State Environmental Protection Key Laboratory of Simulation and Control of Groundwater Pollution, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
c.
Beijing Key Laboratory of Aqueous Typical Pollutants Control and Water Quality Safeguard, School of Environmental, Beijing Jiaotong University, Beijing 100044, China
d.
College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China
e.
Institute of Carbon Neutrality, Zhejiang Wanli University, Ningbo 315100, China

boru3472016@163.com

zhangqr@ysu.edu.cn

Received Date: 29 November 2024
Revised Date: 6 February 2025
Accepted Date: 20 March 2025
Available Online: 21 March 2025

Figures(5)

Successfully generating reactive oxygen species (ROS) in a targeted and efficient manner for the detoxification of chlorinated organic pollutants (CPs) is a significant and demanding challenge. Herein, we present an in-situ photoreduction strategy to fabricate a composite of palladium (Pd) nanoparticles anchored few-layer carbon nitride nanosheets (Pd-CN). This innovative Pd-CN is then leveraged to activate peroxymonosulfate (PMS) in pursuit of our objective. The incorporation of Pd nanoparticles enhances PMS absorption and targets its terminal oxygen, thereby aiding in the cleavage of the O-O bond. This process generates crucial intermediates, including adsorbed hydroxyl radicals (^*OH) and adsorbed atomic oxygen (O^*), which are essential for the production of ¹O₂. Consequently, the Pd-CN catalyst demonstrates strong preference for ¹O₂ generation during the PMS activation process, successfully degrading over 95% of pollutants such as 4-chlorophenol (4-CP), 2,4-dichlorophenol (2,4-DCP), and 2,4,6-trichlorophenol (2,4,6-TCP) within just 20 min. Additionally, the catalyst exhibits total organic carbon (TOC) removal rates ranging from 49.4% to 31.4%, while the rates for de-chlorination fall between 68.6% and 72.7%. A subsequent continuous-flow treatment experiment has confirmed the application potential of this system, demonstrating consistent catalytic activity for up to 8 h. This promising technique presents an efficient strategy for addressing the high toxicity of chlorinated organic pollutants in contaminated water.
- Pd species,
- Few-layer carbon nitride,
- Peroxymonosulfate,
- Singlet oxygen,
- Chlorinated organic pollutants
1. [1]
  K. Zhao, X. Quan, Y. Su, et al., Environ. Sci. Technol. 55 (2021) 14194–14203. doi: 10.1021/acs.est.1c04943
2. [2]
  J.Y. Sun, S. Garg, T.D. Waite, Environ. Sci. Technol. 58 (2024) 13131–13144. doi: 10.1021/acs.est.4c03842
3. [3]
  M. Lei, Q. Gao, K.M. Zhou, et al., Sep. Purif. Technol. 257 (2021) 117933. doi: 10.1016/j.seppur.2020.117933
4. [4]
  Z.N. Garba, W.M. Zhou, I. Lawan, et al., J. Environ. Manage. 241 (2019) 59–75. doi: 10.1016/j.jenvman.2019.04.004
5. [5]
  B.R. Gao, L.R. Wu, S.K. Li, et al., J. Hazard. Mater. 483 (2025) 136698. doi: 10.1016/j.jhazmat.2024.136698
6. [6]
  T.Y. Wu, Y.J. Zuo, H. Chen, Z.Y. Xu, S.R. Zheng, Appl. Catal A: Gen. 666 (2023) 119407. doi: 10.1016/j.apcata.2023.119407
7. [7]
  C. Descorme, Catal. Today 297 (2017) 324–334. doi: 10.1016/j.cattod.2017.03.039
8. [8]
  T.G. Ma, M.J. Liu, N.A.O. Offiong, et al., J. Hazard. Mater. 445 (2023) 130580. doi: 10.1016/j.jhazmat.2022.130580
9. [9]
  S.L. Wang, M.R. Razanajatovo, X.D. Du, et al., Chin. Chem. Lett. 35 (2024) 109140. doi: 10.1016/j.cclet.2023.109140
10. [10]
  M.M. Ao, J. Wei, C.S. He, et al., Chin. Chem. Lett. 36 (2025) 109882. doi: 10.1016/j.cclet.2024.109882
11. [11]
  K.C. Yang, Y.X. Zhao, M. Ji, et al., Water Res. 193 (2021) 116862. doi: 10.1016/j.watres.2021.116862
12. [12]
  S.A.C. Lima, M.F.J. Raposo, P.M.L. Castro, R.M. Morais, Water Res. 38 (2004) 97–102. doi: 10.1016/j.watres.2003.09.005
13. [13]
  T.G. Ma, M.J. Liu, T.T. Li, H.J. Ren, R. Zhou, Sep. Purif. Technol. 293 (2022) 121124. doi: 10.1016/j.seppur.2022.121124
14. [14]
  Y. Zhao, L. Yu, C.Y. Song, et al., Environ. Sci. Technol. 56 (2022) 10710–10720. doi: 10.1021/acs.est.2c01759
15. [15]
  L.S. Zhang, X.H. Jiang, Z.A. Zhong, et al., Angew. Chem. Int. Ed. 60 (2021) 21751–21755. doi: 10.1002/anie.202109488
16. [16]
  G.Y. Bi, R.R. Ding, J.S. Song, et al., Angew. Chem. Int. Ed. 63 (2024) e202401551.
17. [17]
  Q.Q. Tang, B.X. Wu, X.W. Huang, et al., Nat. Commun. 15 (2024) 9549. doi: 10.1038/s41467-024-53941-8
18. [18]
  Z.W. Wang, E. Almatrafi, H. Wang, et al., Angew. Chem. Int. Ed. 61 (2022) e202202338. doi: 10.1002/anie.202202338
19. [19]
  X.Y. Mi, P.F. Wang, S.Z. Xu, et al., Angew. Chem. Int. Ed. 60 (2021) 4588–4593. doi: 10.1002/anie.202014472
20. [20]
  H.Y. Zhuo, X. Zhang, J.X. Liang, et al., Chem. Rev. 120 (2020) 12315–12341. doi: 10.1021/acs.chemrev.0c00818
21. [21]
  C.Y. Dong, Z.R. Gao, Y.L. Li, et al., Nat. Catal. 5 (2022) 485–493. doi: 10.1038/s41929-022-00769-4
22. [22]
  Y.N. Wu, S. Wu K. Zhao, et al., Environ. Sci. Technol. 58 (2024) 20699–20709. doi: 10.1021/acs.est.4c06064
23. [23]
  K. Cheng, L.C.J. Smulders, L.I. van der Wal, et al., Science 377 (2022) 204–208. doi: 10.1126/science.abn8289
24. [24]
  B. Sheng, C.Y. Deng, Y.F. Li, et al., ACS Catal. 12 (2022) 14679–14688. doi: 10.1021/acscatal.2c04484
25. [25]
  Y.Y. Yao, C.H. Wang, X. Yan, et al., Environ. Sci. Technol. 56 (2022) 8833–8843. doi: 10.1021/acs.est.2c00706
26. [26]
  Z. Cai, Y.M. Bi, E.Y. Hu, et al., Adv. Energy. Mater. 8 (2018) 1701694. doi: 10.1002/aenm.201701694
27. [27]
  Y.B. Wang, D. Cao, M. Liu, X. Zhao, Catal. Commun. 102 (2017) 85–88. doi: 10.1016/j.catcom.2017.08.016
28. [28]
  D.E. Eastman, Phys. Rev. B 2 (1970) 1.
29. [29]
  J. Deng, F.Z. Li, Z. Qi, et al., Appl. Catal. B: Environ. Energy 359 (2024) 124499. doi: 10.1016/j.apcatb.2024.124499
30. [30]
  F. Ye, J. Qian, J.J. Xia, et al., Environ. Res. 249 (2024) 118497. doi: 10.1016/j.envres.2024.118497
31. [31]
  X. Long, W.Q. Chen, C. Lei, et al., Sci. Total. Environ. 775 (2021) 145178. doi: 10.1016/j.scitotenv.2021.145178
32. [32]
  Z.J. Li, Z.Y. Guo, X.Y. Wu, et al., ACS Nano 17 (2023) 22859–22871. doi: 10.1021/acsnano.3c07724
33. [33]
  J. Wang, B. Li, Y. Li, et al., Adv. Sci. 8 (2021) 202101824.
34. [34]
  Q.Z. Fang, H.L. Yang, S.J. Ye, et al., Water Res. 245 (2023) 120614. doi: 10.1016/j.watres.2023.120614
35. [35]
  T. Entradas, S. Waldron, M. Volk, J. Photoch. Photobio. B 204 (2020) 111787. doi: 10.1016/j.jphotobiol.2020.111787
36. [36]
  P.H. Shao, Y.P. Jing, X.G. Duan, et al., Environ. Sci. Technol. 55 (2021) 16078–16087. doi: 10.1021/acs.est.1c02042
37. [37]
  M.Z. Hu, J.Y. Zhu, W.J. Zhou, Environ. Pollut. 270 (2021) 116092. doi: 10.1016/j.envpol.2020.116092
38. [38]
  H.Z. Liu, X.X. Shu, M.J. Huang, et al., Nat. Commun. 15 (2024) 2327. doi: 10.1038/s41467-024-46739-1
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2. [2]
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3. [3]
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4. [4]
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6. [6]
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沈阳化工大学材料科学与工程学院沈阳 110142