Citation: Chunhe Cao, Wenwen Zheng, Suhang Meng, Qiuyu Rong, Yi Li. Synergistic Fe single-atom and nanoparticle dual-site catalysis in electrocatalytic system for enhanced H₂O₂ adsorption and activation[J]. Chinese Chemical Letters, ;2026, 37(11): 112570. doi: 10.1016/j.cclet.2026.112570 shu

Synergistic Fe single-atom and nanoparticle dual-site catalysis in electrocatalytic system for enhanced H₂O₂ adsorption and activation

Chunhe Cao ^{a, 1} ,
Wenwen Zheng ^{c, 1} ,
Suhang Meng ^a ,
Qiuyu Rong ^a ,
Yi Li ^{a, b, *,}

a.
Key Laboratory of Organic Integrated Circuits, Ministry of Education & Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University, Tianjin 300072, China
b.
Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, China
c.
China National Offshore Oil Corporation, Tianjin Branch, Tianjin 300452, China

liyi@tju.edu.cn

Received Date: 16 September 2025
Revised Date: 10 December 2025
Accepted Date: 2 March 2026
Available Online: 3 March 2026

Figures(6)

The efficiency of in-situ production of H₂O₂ from O₂ and subsequent conversion of H₂O₂ into reactive oxygen species (ROS) in the electro-Fenton (EF) system is a key limiting factor for its widespread application in practical water treatment. To address this key issue, we propose a design strategy based on the synergistic interaction between iron single-atom catalysts (SACs) and iron nanoparticles (PCs). The introduction of Fe⁰/Fe₇C₃ PCs not only significantly accelerates the redox cycle of iron species and enhances electron transfer efficiency, but also precisely induces an asymmetric redistribution of electrons around the Fe SACs, increasing the electron cloud density. This electron enrichment subsequently enhances the adsorption capacity of H₂O₂ at the active sites and thereby improving its activation efficiency. Experimental results show that the incorporation of Fe PCs increases the first-order kinetic constant of Fe_SAC-PC@NC to 3.8 times that of Fe_SAC@NC, and the degradation efficiency for various pollutants exceeds 93%. Moreover, the catalyst maintains excellent stability and performance under continuous degradation tests and scaled-up experiment, with an energy efficiency of oxidation (E_EO) as low as 3.7 kWh/m³, highlighting its promising potential for industrial application. This study demonstrates that the synergistic strategy of Fe SACs and Fe⁰/Fe₇C₃ PCs provides a research direction and technical pathway for enhancing H₂O₂ activation efficiency in the EF system.
- H₂O₂ activation,
- Dual-site catalysis,
- Electro-Fenton system,
- ¹O₂,
- N-doped biochar
1. [1]
  M.R. Wang, B.L. Bodirsky, R. Rijneveld, et al., Nat. Commun. 15 (2024) 880. doi: 10.1038/s41467-024-44947-3
2. [2]
  Z.Y. Zhao, Y.N. Mi, S.L. Wang, X.D. Du, Q.R. Zhang, Water Res. 280 (2025) 123510. doi: 10.1016/j.watres.2025.123510
3. [3]
  M. Hassan, H. Olvera-Vargas, X.P. Zhu, B. Zhang, Y.L. He, J. Power Sources 424 (2019) 220–244. doi: 10.1016/j.jpowsour.2019.03.112
4. [4]
  S.L. Wang, M.R. Razanajatovo, X.D. Du, et al., Chin. Chem. Lett. 35 (2024) 109140. doi: 10.1016/j.cclet.2023.109140
5. [5]
  S. Wang, S.M. Guo, X.D. Du, et al., Chem. Eng. J. 495 (2024) 153604. doi: 10.1016/j.cej.2024.153604
6. [6]
  J.Y. Yu, Y. Cheng, A.H. Cai, et al., Chin. Chem. Lett. 36 (2025) 110549. doi: 10.1016/j.cclet.2024.110549
7. [7]
  Y. Jiang, J.B. Ran, K. Mao, et al., Ecotoxicol. Environ. Saf. 236 (2022) 113464. doi: 10.1016/j.ecoenv.2022.113464
8. [8]
  H.Y. Sheng, A.N. Janes, R.D. Ross, et al., Energy Environ. Sci. 13 (2020) 4189–4203. doi: 10.1039/D0EE01925A
9. [9]
  F. Miao, M.M. Gao, X. Yu, et al., Electrochem. Commun. 113 (2020) 106687. doi: 10.1016/j.elecom.2020.106687
10. [10]
  X.L. Zhang, C.Y. Wu, Z.H. Wang, et al., Environ. Res. 263 (2024) 120020. doi: 10.1016/j.envres.2024.120020
11. [11]
  Z.H. Chen, D. Yan, X.S. Wang, et al., ACS Catal. 15 (2025) 13568–13580. doi: 10.1021/acscatal.5c02889
12. [12]
  Z.P. Lou, M.T. Liu, D.Y. Tang, et al., Appl. Catal. B: Environ. 315 (2022) 121523. doi: 10.1016/j.apcatb.2022.121523
13. [13]
  H.F. Chan, Q. Du, C.L. Yue, et al., Appl. Catal. B: Environ. 382 (2026) 125953. doi: 10.1016/j.apcatb.2025.125953
14. [14]
  M. Tian, Y.Z. Zhu, D.L. Zhang, et al., Nano Energ. 64 (2019) 103940. doi: 10.1016/j.nanoen.2019.103940
15. [15]
  S. Kabir, K. Artyushkova, A. Serov, P. Atanassov, ACS Appl. Mater. Interfaces 10 (2018) 11623–11632. doi: 10.1021/acsami.7b18651
16. [16]
  J.L. Li, W.W. Zheng, S.H. Meng, et al., Adv. Funct. Mater. 35 (2025) 2417538. doi: 10.1002/adfm.202417538
17. [17]
  H.P. Rong, S.F. Ji, J.T. Zhang, D.S. Wang, Y.D. Li, Nat. Commun. 11 (2020) 5884. doi: 10.1038/s41467-020-19571-6
18. [18]
  Y. Wang, X.B. Zheng, D.S. Wang, Nano Res. 15 (2022) 1730–1752. doi: 10.1007/s12274-021-3794-0
19. [19]
  S.F. Ji, B. Jiang, H.G. Hao, et al., Nat. Catal. 4 (2021) 407–417. doi: 10.1038/s41929-021-00609-x
20. [20]
  J.R. Yang, W.H. Li, D.S. Wang, Chem. Catal. 1 (2021) 24–26.
21. [21]
  Z.C. Zhuang, Y. Li, Y.H. Li, et al., Energy Environ. Sci. 14 (2021) 1016–1028. doi: 10.1039/D0EE03701J
22. [22]
  H.Y. Jing, Z.Y. Zhao, C.Y. Zhang, et al., Nano Res. 14 (2021) 4025–4032. doi: 10.1007/s12274-021-3331-1
23. [23]
  D. Zhou, L.L. Zhang, X.Y. Liu, et al., Nano Res. 15 (2022) 519–527. doi: 10.1007/s12274-021-3511-z
24. [24]
  L.C. Liu, D.M. Meira, R. Arenal, et al., ACS Catal. 9 (2019) 10626–10639. doi: 10.1021/acscatal.9b04214
25. [25]
  C. Mu, Z.H. Liu, Q.F. Yao, Q. He, J.P. Xie, SmartMat 6 (2025) e1317. doi: 10.1002/smm2.1317
26. [26]
  X. Guo, H. Zhang, Y.L. Wang, et al., Angew. Chem. Int. Ed. 64 (2025) e202511266. doi: 10.1002/anie.202511266
27. [27]
  Z.R. Zhou, Y.N. Li, M.M. Li, Y. Li, S.H. Zhan, Chin. Chem. Lett. 31 (2020) 2698–2704. doi: 10.1016/j.cclet.2020.07.003
28. [28]
  J.L. Li, Y.P. Liu, S.H. Meng, et al., ACS ES&T Water 4 (2024) 5868–5879.
29. [29]
  H.Y. Gang, H.Y. Deng, L. Yan, et al., J. Colloid Interface Sci. 638 (2023) 252–262. doi: 10.1016/j.jcis.2023.01.093
30. [30]
  Y.J. Ji, F.Y. Xu, K. Fang, et al., Environ. Technol. Innov. 38 (2025) 104079. doi: 10.1016/j.eti.2025.104079
31. [31]
  S.H. Meng, J.L. Li, S.Y. Wang, et al., Adv. Mater. 37 (2025) 2420080. doi: 10.1002/adma.202420080
32. [32]
  C. Xia, S. Back, S. Ringe, et al., Nat. Catal. 3 (2020) 125–134. doi: 10.1038/s41929-019-0402-8
33. [33]
  Y.P. Liu, P.F. Wang, L.B. Xie, et al., Angew. Chem. Int. Ed. 63 (2024) e202319470. doi: 10.1002/anie.202319470
34. [34]
  X.Y. Lu, D. Wang, K.H. Wu, X.L. Guo, W. Qi, J. Colloid Interface Sci. 573 (2020) 376–383. doi: 10.1016/j.jcis.2020.04.030
35. [35]
  W. Wang, Y.X. Zheng, Y.C. Hu, Y.C. Liu, S.L. Chen, J. Phys. Chem. Lett. 13 (2022) 8914–8920. doi: 10.1021/acs.jpclett.2c02684
36. [36]
  C.C.L. McCrory, S. Jung, J.C. Peters, T.F. Jaramillo, J. Am. Chem. Soc. 135 (2013) 16977–16987. doi: 10.1021/ja407115p
37. [37]
  Y. Tong, J.C. Wu, P.Z. Chen, et al., J. Am. Chem. Soc. 140 (2018) 11165–11169. doi: 10.1021/jacs.8b06108
38. [38]
  F. Ye, Y. Liu, Q.R. Lv, et al., Chin. Chem. Lett. 37 (2026) 111136. doi: 10.1016/j.cclet.2025.111136
39. [39]
  X.M. Chen, Y.Y. Wu, Y. Tang, et al., Chin. Chem. Lett. 35 (2024) 109245. doi: 10.1016/j.cclet.2023.109245
40. [40]
  X. Huang, M. Song, J. Zhang, et al., Nano Res. 15 (2022) 3927–3932. doi: 10.1007/s12274-021-4057-9
41. [41]
  L.L. Wang, X. Lan, W.Y. Peng, Z.H. Wang, J. Hazard. Mater. 408 (2021) 124436. doi: 10.1016/j.jhazmat.2020.124436
42. [42]
  P. Chen, E.I. Solomon, Proc. Natl. Acad. Sci. U. S. A. 101 (2004) 13105–13110. doi: 10.1073/pnas.0402114101
43. [43]
  N. Mahne, B. Schafzahl, C. Leypold, et al., Nat. Energy 2 (2017) 17036. doi: 10.1038/nenergy.2017.36
44. [44]
  F. Xiao, Z.N. Wang, J.Q. Fan, et al., Angew. Chem. Int. Ed. 60 (2021) 10375–10383. doi: 10.1002/anie.202101804
45. [45]
  X.M. Xu, Y.M. Zhang, Y. Chen, et al., Proc. Natl. Acad. Sci. U. S. A. 119 (2022) e2205562119. doi: 10.1073/pnas.2205562119
46. [46]
  Z.C. Yang, J.S. Qian, A.Q. Yu, B.C. Pan, Proc. Natl. Acad. Sci. U. S. A. 116 (2019) 6659–6664. doi: 10.1073/pnas.1819382116
47. [47]
  A.U. Khan, M. Kasha, Proc. Natl. Acad. Sci. U. S. A. 91 (1994) 12365–12367. doi: 10.1073/pnas.91.26.12365
48. [48]
  X.F. Feng, R.X. Long, C.C. Liu, Y. Lu, X.B. Liu, Chem. Eng. J. 471 (2023) 144447. doi: 10.1016/j.cej.2023.144447
49. [49]
  J.L. Zheng, Q.T. Lin, Y.X. Liu, et al., Chem. Eng. J. 452 (2023) 139233. doi: 10.1016/j.cej.2022.139233
50. [50]
  A.V. Mohod, M. Momotko, N.S. Shah, et al., Water Resour. Ind. 30 (2023) 100220. doi: 10.1016/j.wri.2023.100220
51. [51]
  S. Li, X.R. Liu, Y.J. Zheng, et al., Chin. Chem. Lett. 35 (2024) 108971. doi: 10.1016/j.cclet.2023.108971
52. [52]
  S.Y. Hou, H.L. Hu, Q. Fu, et al., Sep. Purif. Technol. 333 (2024) 125980. doi: 10.1016/j.seppur.2023.125980
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Synergistic Fe single-atom and nanoparticle dual-site catalysis in electrocatalytic system for enhanced H2O2 adsorption and activation

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Synergistic Fe single-atom and nanoparticle dual-site catalysis in electrocatalytic system for enhanced H₂O₂ adsorption and activation