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Universal complexing agent enabling advanced iron-cerium redox flow batteries
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  • Published: 31 December 2025

Universal complexing agent enabling advanced iron-cerium redox flow batteries

  • Jiahui Yang1,2,
  • Wei Wei3,
  • Chengxi Zhou1,
  • Xinyi Tan4,
  • Tai-Sing Wu  ORCID: orcid.org/0000-0002-3285-72585,
  • Yi Zhang6,
  • Yun-Liang Soo  ORCID: orcid.org/0000-0002-1683-31417,
  • Molly Meng-Jung Li  ORCID: orcid.org/0000-0001-7197-97016,
  • Alex W. Robertson  ORCID: orcid.org/0000-0002-9521-64828,
  • Ao Tang3 &
  • …
  • Zhenyu Sun  ORCID: orcid.org/0000-0001-5788-93391 

Nature Communications , Article number:  (2025) Cite this article

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We are providing an unedited version of this manuscript to give early access to its findings. Before final publication, the manuscript will undergo further editing. Please note there may be errors present which affect the content, and all legal disclaimers apply.

Subjects

  • Batteries
  • Energy

Abstract

The development of a safe and affordable redox flow battery technology is important for storing intermittent renewable energy. Here, we design a stable aqueous organic iron-cerium redox flow battery based on the inexpensive metal iron and the abundant rare earth metal cerium, enabled by the universal complexing agent diethylenetriamine pentaacetic acid. Molecular dynamics simulations are employed to screen for carboxyl-containing ligands with different electron donating capacities, revealing that diethylenetriamine pentaacetic acid is an effective candidate to chelate iron and cerium in the negolyte and posolyte, respectively, as verified by experimental characterization. The complexing agent enhances the redox characteristics of iron and cerium and reduces osmotic water migration between the negative and positive chambers by allowing the same ligand in both electrolytes. Our iron-cerium redox flow battery achieves an energy efficiency of 87.7% at 40 mA cm−2 and 80.6% at 100 mA cm−2, while retaining 95.3% of its initial capacity and maintaining around 86.3% energy efficiency after 500 cycles under neutral environments (100% of state-of-charge). The capacity is still preserved after 1779 cycles even when cycled at high-rates (80 mA·cm−2, 70% of state-of-charge).

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Data availability

The data generated in this study are provided in the Supplementary Information/Source Data file. Source data are provided with this paper.

References

  1. Carrington, M. E. et al. Associative pyridinium electrolytes for air-tolerant redox flow batteries. Nature 623, 949–955 (2023).

    Google Scholar 

  2. Ai, F. et al. Heteropoly acid negolytes for high-power-density aqueous redox flow batteries at low temperatures. Nat. Energy 7, 417–426 (2022).

    Google Scholar 

  3. Feng, R. et al. Reversible ketone hydrogenation and dehydrogenation for aqueous organic redox flow batteries. Science 372, 836–840 (2021).

    Google Scholar 

  4. Robb, B. H., Farrell, J. M. & Marshak, M. P. Chelated chromium electrolyte enabling high-voltage aqueous flow batteries. Joule 3, 2503–2512 (2019).

    Google Scholar 

  5. Waters, S. E., Davis, C. M., Thurston, J. R. & Marshak, M. P. Maximizing vanadium deployment in redox flow batteries through chelation. J. Am. Chem. Soc. 144, 17753–17757 (2022).

    Google Scholar 

  6. Scott, E. W., Brian, H. R. & Michael, P. M. Effect of chelation on iron–chromium redox flow batteries. ACS Energy Lett 5, 1758–1762 (2020).

    Google Scholar 

  7. Park, M., Ryu, J., Wang, W. & Cho, J. Material design and engineering of next-generation flow-battery technologies. Nature Rev. Mater. 2, 16080 (2016).

    Google Scholar 

  8. Zhao, Z. et al. Development of flow battery technologies using the principles of sustainable chemistry. Chem. Soc. Rev. 52, 6031–6074 (2023).

    Google Scholar 

  9. Zhang, X., Li, W. & Chen, H. High-capacity CuSi2P3-based semisolid anolyte for redox flow batteries. ACS Appl. Mater. Interfaces 13, 40552–40561 (2021).

    Google Scholar 

  10. Zhi, L. et al. New alkalescent electrolyte chemistry for zinc-ferricyanide flow battery. Angew. Chem. Int. Ed. 63, e202403607 (2024).

    Google Scholar 

  11. Yu, Z. et al. Electrolyte engineering for efficient and stable vanadium redox flow batteries. Energy Storage Mater 69, 103404 (2024).

    Google Scholar 

  12. Xing, F. et al. Highly active hollow porous carbon spheres@graphite felt composite electrode for high power density vanadium flow batteries. Adv. Funct. Mater. 32, 2111267 (2022).

    Google Scholar 

  13. Agarwal, H. et al. Electrode treatments for redox flow batteries: translating our understanding from vanadium to aqueous-organic. Adv. Sci. 11, e2307209 (2024).

    Google Scholar 

  14. Wei, J. et al. Energy density boosted vanadium colloid flow batteries realized by a reversible nanoparticle suspension-dissolution strategy. Adv. Funct. Mater. 34, 2314956 (2024).

    Google Scholar 

  15. Zhu, F., Guo, W. & Fu, Y. Functional materials for aqueous redox flow batteries: merits and applications. Chem. Soc. Rev. 52, 8410–8446 (2023).

    Google Scholar 

  16. Zhang, S. et al. Regulated adsorption capability by interface-electric-field enabling promoted electrochemical kinetics of zinc-bromine flow batteries. Chem. Eng. J. 486, 150317 (2024).

    Google Scholar 

  17. Huang, K. et al. Porous ceramic metal-based flow battery composite membrane. Angew. Chem. Int. Ed. 63, e202401558 (2024).

    Google Scholar 

  18. Wei, X. et al. Materials and systems for organic redox flow batteries: status and challenges. ACS Energy Lett 2, 2187–2204 (2017).

    Google Scholar 

  19. Jang, J. E. et al. Full-hexacyanometallate aqueous redox flow batteries exceeding 1.5 V in an aqueous solution. Adv. Energy Mater. 13, 2300707 (2023).

    Google Scholar 

  20. Li, X. et al. A complexing agent to enable a wide-temperature range bromine-based flow battery for stationary energy storage. Adv. Funct. Mater. 31, 2100133 (2021).

    Google Scholar 

  21. Ling, R. et al. Dual-function electrolyte additive design for long-life alkaline zinc flow batteries. Adv. Mater. 36, e2404834 (2024).

    Google Scholar 

  22. Kwabi, D. G. Molecular engineering expands the chemical possibilities for organic flow batteries. Joule 5, 1636–1638 (2021).

    Google Scholar 

  23. Sun, J., Shi, D., Zhong, H., Li, X. & Zhang, H. Investigations on the self-discharge process in vanadium flow battery. J. Power Sources 294, 562–568 (2015).

    Google Scholar 

  24. Chou, Y.-S., Devi, N., Yen, S.-C., Singh, P. & Chen, Y.-S. Study on the self-discharge of an all-vanadium redox flow battery through monitoring individual cell voltages. ACS Sustainable Chem. Eng. 10, 12245–12251 (2022).

    Google Scholar 

  25. Hruska, L. W. & Savinell, R. F. Investigation of factors affecting performance of the iron-redox battery. J. Electrochem. Soc. 128, 18–25 (1981).

    Google Scholar 

  26. Noh, C., Chung, Y. & Kwon, Y. Organometallic redox flow batteries using iron triethanolamine and cobalt triethanolamine complexes. J. Power Sources 466, 228333 (2020).

    Google Scholar 

  27. Shin, M., Noh, C., Chung, Y. & Kwon, Y. All-iron aqueous redox flow batteries using organometallic complexes consisting of iron and 3-bis(2-hydroxyethyl)amino-2-hydroxypropanesulfonic acid ligand and ferrocyanide as redox couple. Chem. Eng. J. 398, 125631 (2020).

    Google Scholar 

  28. Shin, M., Noh, C. & Kwon, Y. Stability enhancement for all-iron aqueous redox flow battery using iron-3-[bis(2-hydroxyethyl)amino]-2-hydroxypropanesulfonic acid complex and ferrocyanide as redox couple. Int. J. Energy Res. 46, 6866–6875 (2021).

    Google Scholar 

  29. Nambafu, G. S. et al. Phosphonate-based iron complex for a cost-effective and long cycling aqueous iron redox flow battery. Nat. Commun. 15, 2566 (2024).

    Google Scholar 

  30. Gong, K. et al. All-soluble all-iron aqueous redox-flow battery. ACS Energy Lett 1, 89–93 (2016).

    Google Scholar 

  31. Yang, J. et al. High-stable all-iron redox flow battery with innovative anolyte based on steric hindrance regulation. Angew. Chem. Int. Ed. 64, e202414452 (2025).

    Google Scholar 

  32. Xie, X., Mushtaq, F., Wang, Q. & Daoud, W. A. The renaissance of the Zn–Ce flow battery: dual-membrane configuration enables unprecedentedly high efficiency. ACS Energy Lett 7, 3484–3491 (2022).

    Google Scholar 

  33. Modiba, P., Matoetoe, M. & Crouch, A. M. Electrochemical impedance spectroscopy study of Ce(IV) with aminopolycarboxylate ligands for redox flow battery applications. J. Power Sources 205, 1–9 (2012).

    Google Scholar 

  34. Schmickler, W., Nazmutdinov, R. R., Wang, Q. & Daoud, W. A. Electrochemistry of Ce(IV)/Ce(III) redox couples in mixed solutions for aqueous flow battery: Experimental and molecular modelling study. Electrochim. Acta 368, 137601 (2021).

    Google Scholar 

  35. Leung, P. K., Ponce-de-León, C. & Walsh, F. C. The influence of operational parameters on the performance of an undivided zinc-cerium flow battery. Electrochim. Acta 80, 7–14 (2012).

    Google Scholar 

  36. Song, Y. et al. Electrolyte transfer mechanism and optimization strategy for vanadium flow batteries adopting a Nafion membrane. J. Power Sources 449, 227503 (2020).

    Google Scholar 

  37. Leung, P. K., Ponce-de-León, C., Low, C. T. J., Shah, A. A. & Walsh, F. C. Characterization of a zinc–cerium flow battery. J. Power Sources 196, 5174–5185 (2011).

    Google Scholar 

  38. Li, Y. et al. Cerium-containing complexes for low-cost, non-aqueous redox flow batteries (RFBs). J. Power Sources 450, 227634 (2020).

    Google Scholar 

  39. Yu, H., Pritzker, M. & Gostick, J. Use of Mixed methanesulfonic acid/sulfuric acid as positive supporting electrolyte in Zn–Ce redox flow battery. J. Electrochem. Soc. 170, 020536 (2023).

    Google Scholar 

  40. Na, Z., Yao, R., Yan, Q., Sun, X. & Huang, G. General growth of carbon nanotubes for cerium redox reactions in high-efficiency redox flow batteries. Res 2019, 3616178 (2019).

    Google Scholar 

  41. Na, Z., Wang, X., Liu, X., Li, W. & Sun, X. O/N/S trifunctional doping on graphite felts: A novel strategy toward performance boosting of cerium-based redox flow batteries. Carbon Energy 3, 752–761 (2021).

    Google Scholar 

  42. Wu, Y. et al. A green europium-cerium redox flow battery with ultrahigh voltage and high performance. Chem. Eng. J. 500, 157189 (2024).

    Google Scholar 

  43. Kocyigit, N., Gencten, M., Sahin, M. & Sahin, Y. A novel electrolyte for redox flow batteries: Cerium and chromium couples in an aqueous system. Int. J. Energy Res. 45, 16176–16188 (2021).

    Google Scholar 

  44. Na, Z., Xu, S., Yin, D. & Wang, L. A cerium–lead redox flow battery system employing a supporting electrolyte of methanesulfonic acid. J. Power Sources 295, 28–32 (2015).

    Google Scholar 

  45. Leung, P. K., Ponce-de-León, C. & Walsh, F. C. An undivided zinc–cerium redox flow battery operating at room temperature (295 K). Electrochem. Commun. 13, 770–773 (2011).

    Google Scholar 

  46. Wu, J. et al. Boosting the kinetics of Ce3+/Ce4+ redox reaction by constructing TiC/TiO2 heterojunction for cerium-based flow batteries. Adv. Funct. Mater. 34, 2309825 (2023).

    Google Scholar 

  47. Chang, T. C. et al. Cerium/ascorbic acid/iodine active species for redox flow energy storage battery. Molecules 26, 3443 (2021).

    Google Scholar 

Download references

Acknowledgments

This work was supported by the National Natural Science Foundation of China (22372007 and 21972010) and the Joint Funds of the National Natural Science Foundation of China (U24B20201).

Author information

Authors and Affiliations

  1. State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, 100029, PR China

    Jiahui Yang, Chengxi Zhou & Zhenyu Sun

  2. National Institute of Clean-and-Low-Carbon Energy, Beijing, 102211, PR China

    Jiahui Yang

  3. Institute of Metal Research Chinese Academy of Sciences, Shenyang, 110016, PR China

    Wei Wei & Ao Tang

  4. School of Materials Science and Engineering, Beijing Institute of Technology, Beijing Key Laboratory of Environmental Science and Engineering, Beijing, 100081, PR China

    Xinyi Tan

  5. National Synchrotron Radiation Research Center, Hsinchu, 30076, Taiwan

    Tai-Sing Wu

  6. Department of Applied Physics, The Hong Kong Polytechnic University, Hong Kong, PR China

    Yi Zhang & Molly Meng-Jung Li

  7. Department of Physics, National Tsing Hua University, Hsinchu, 30013, Taiwan

    Yun-Liang Soo

  8. Department of Physics, University of Warwick, Coventry, CV4 7AL, UK

    Alex W. Robertson

Authors
  1. Jiahui Yang
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  2. Wei Wei
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Contributions

J.Y. designed and performed most of the experiments and wrote the draft. W.W. and A.T. conducted the calculations. C.Z. helped perform some battery measurements. T.W., Y.Z., Y.S., and M.L. carried out XAFS measurements and analyses. A.R. helped polish the language. X.T., A.T., and Z.S. revised the manuscript. Z.S. supervised the project.

Corresponding authors

Correspondence to Xinyi Tan, Ao Tang or Zhenyu Sun.

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Nature Communications thanks Juezhi Yu and the other anonymous reviewer(s) for their contribution to the peer review of this work. A peer review file is available.

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Supplementary Data 1

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Yang, J., Wei, W., Zhou, C. et al. Universal complexing agent enabling advanced iron-cerium redox flow batteries. Nat Commun (2025). https://doi.org/10.1038/s41467-025-67878-z

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  • Received: 07 February 2025

  • Accepted: 11 December 2025

  • Published: 31 December 2025

  • DOI: https://doi.org/10.1038/s41467-025-67878-z

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