Issue

Vol. 18 (2026)

Dual-Site Functional Orchestration Enables Synergistic Anodic Modulation and Cathodic Mooring for Durable Zinc–Iodine Batteries

https://doi.org/10.1007/s40820-026-02144-5
Yan Jin
College of Materials and Chemical Engineering, China Three Gorges University, Yichang 443002, Hubei, People’s Republic of China
Jin Cao
College of Materials and Chemical Engineering, China Three Gorges University, Yichang 443002, Hubei, People’s Republic of China
Can Huang
College of Materials and Chemical Engineering, China Three Gorges University, Yichang 443002, Hubei, People’s Republic of China
Xin An
College of Materials and Chemical Engineering, China Three Gorges University, Yichang 443002, Hubei, People’s Republic of China
Shenghan Wang
College of Materials and Chemical Engineering, China Three Gorges University, Yichang 443002, Hubei, People’s Republic of China
Xuelin Yang
Institute of Energy Storage Technology, China Three Gorges University, Yichang 443002, Hubei, People’s Republic of China

Corresponding Author: Xuelin Yang

xlyang@ctgu.edu.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 301

Abstract

Aqueous zinc-iodine batteries represent a compelling technology for large-scale, sustainable energy storage, yet their practical application is severely hampered by the simultaneous interfacial challenges of uncontrolled dendrite growth on the zinc anode and the parasitic polyiodide shuttle. Herein, we introduce a dual-site functional orchestration strategy by employing a single electrolyte additive, 2-imidazolidone (ELA), to concurrently stabilize both the anode and cathode interfaces. On the anode side, the carbonyl (C=O) functional group of ELA initiates an effective anodic modulation, regulating the Zn2+ solvation environment and facilitating a dynamic adsorption layer. This homogenizes the ion flux and guides preferential Zn deposition along the (002) plane, effectively suppressing dendrite formation. Concurrently, at the cathode, the imino (N-H) group immobilizes soluble polyiodide species via hydrogen bonding, realizing an effective cathodic mooring. This targeted confinement arrests the shuttle effect without impeding the intrinsic redox kinetics. This synergistic stabilization translates into exceptional electrochemical performance, with symmetric cells achieving an ultra-long lifespan of over 5500 h at a high current density of 8 mA cm-2 and the full Zn||I2 cells demonstrating robust cycling with 79.4% capacity retention after 2500 cycles. This work introduces a dual-site functional orchestration strategy, offering a pathway toward more durable aqueous batteries.


Highlights:
1 A dual-site functional orchestration strategy is proposed using 2-imidazolidone to simultaneously reconfigure the anodic solvation structure and suppress the cathodic polyiodide shuttle.
2 The carbonyl (C=O) group modulates Zn2+ solvation to induce preferred (002) deposition, while the imino (N-H) group chemically moors polyiodides via hydrogen bonding, achieving decoupled synergistic regulation.
3 This molecular engineering enables a record-breaking lifespan exceeding 5500 h at 8 mA cm-2 for Zn anodes and durable full-cell cycling with 79.4% capacity retention over 2500 cycles.

Keywords

Aqueous zinc–iodine batteries Dual-site functional orchestration Interfacial engineering Dendrite suppression Polyiodide shuttle
Jin, Yan, Jin Cao, Can Huang, Xin An, Shenghan Wang, and Xuelin Yang. 2026. “Dual-Site Functional Orchestration Enables Synergistic Anodic Modulation and Cathodic Mooring for Durable Zinc–Iodine Batteries”. Nano-Micro Letters 18 (March):301. https://doi.org/10.1007/s40820-026-02144-5.
Download Citation
Endnote/Zotero/Mendeley (RIS)
BibTeX
References
  1. S. Wang, Z. Wei, H. Hong, X. Guo, Y. Wang et al., A tellurium iodide perovskite structure enabling eleven-electron transfer in zinc ion batteries. Nat. Commun. 16(1), 511 (2025). https://doi.org/10.1038/s41467-024-55385-6
  2. Y. Song, M. Chen, Z. Zhong, Z. Liu, S. Liang et al., Bilateral in-situ functionalization towards Ah-scale aqueous zinc metal batteries. Nat. Commun. 16, 3142 (2025). https://doi.org/10.1038/s41467-025-58153-2
  3. S.-J. Zhang, J. Hao, H. Wu, Y. Hu, Q. Chen et al., Electroactive ferrocene/ferrocenium redox coupling for shuttle-free aqueous zinc-iodine pouch cells. Nat. Chem. 18(2), 266–274 (2026). https://doi.org/10.1038/s41557-025-01986-7
  4. W. Liu, H. Ma, L. Zhao, W. Qian, B. Liu, J. Chen, Y. Yao, Anionically-reinforced nanocellulose separator enables dual suppression of zinc dendrites and polyiodide shuttle for long-cycle Zn-I2 batteries. Nano-Micro Lett. 18(1), 59 (2026). https://doi.org/10.1007/s40820-025-01921-y
  5. D. Li, Y.-J. Zhu, L. Cheng, S. Xie, H.-P. Yu et al., A MXene modulator enabled high-loading iodine composite cathode for stable and high-energy-density Zn-I2 battery. Adv. Energy Mater. 15(12), 2404426 (2025). https://doi.org/10.1002/aenm.202404426
  6. W. Zhang, J. Chen, C. Guan, T. Qiu, X. Shi et al., Harnessing dual hydrogen bonding and lewis acid-base interactions for bio-inspired symmetry-breaking electrolytes in aqueous zinc-ion batteries. Angew. Chem. Int. Ed. 64(43), e202516282 (2025). https://doi.org/10.1002/anie.202516282
  7. W. Zhang, L. He, J. Li, R. Yu, Z. Xu et al., Configurational entropy-tailored NASICON cathode redox chemistry for capacity-dense and ultralong cyclability. Energy Environ. Sci. 18(14), 7278–7290 (2025). https://doi.org/10.1039/d5ee00877h
  8. X. Wei, J. Guan, Y. Mu, Y. Zou, X. Wei, L. Yang, L. Zeng, Decoding hydrogen-bond network of electrolyte for cryogenic durable aqueous zinc-ion batteries. Nano-Micro Lett. 18(1), 127 (2026). https://doi.org/10.1007/s40820-025-01970-3
  9. Q. Fu, W. Zhang, X. Liu, Y. Liu, Z. Lei et al., Dynamic imine chemistry enables paintable biogel electrolytes to shield on-body zinc-ion batteries from interfacial interference. J. Am. Chem. Soc. 146(50), 34950–34961 (2024). https://doi.org/10.1021/jacs.4c14645
  10. J. Cao, X. Rao, S. Qian, D. Zhang, Y. Jin et al., Dynamic Zn2+-coordinating oxygen sites and electric field modulation in boron-integrated cellulose nanofiber separators for stable zinc-ion batteries. Adv. Energy Mater. 15(47), e03368 (2025). https://doi.org/10.1002/aenm.202503368
  11. S. Guo, M. Yao, S. Liang, G. Fang, Failure mechanisms and practical optimizations for ah-scale aqueous zinc-ion pouch cells. Adv. Mater. 37(44), e12364 (2025). https://doi.org/10.1002/adma.202512364
  12. H. Xu, R. Zhang, D. Luo, K. Huang, J. Wang et al., Polarity coupling in biphasic electrolytes enables iodine/polyiodide co-extraction for portable Zn–iodine batteries following a liquid–liquid conversion route. Energy Environ. Sci. 18(15), 7447–7459 (2025). https://doi.org/10.1039/D5EE02593A
  13. J. Cao, H. Wu, D. Zhang, D. Luo, L. Zhang et al., In-situ ultrafast construction of zinc tungstate interface layer for highly reversible zinc anodes. Angew. Chem. Int. Ed. 63(29), e202319661 (2024). https://doi.org/10.1002/anie.202319661
  14. Q. Zong, X. Liu, Q. Zhang, Q. Kang, F. Wang et al., Interfacial gradient engineering synergized with self-adaptive cathodic defense for durable Zn-ion batteries. Energy Environ. Sci. 18(17), 8256–8267 (2025). https://doi.org/10.1039/D5EE02236C
  15. Y. Wang, X. Ma, X. Yang, R. Zhang, H. Hong et al., A multifunctional binder for current-collector-free Zn powder anodes. Adv. Mater. 37(46), 2419702 (2025). https://doi.org/10.1002/adma.202419702
  16. X. Shi, Y. Zhong, Y. Yang, J. Zhou, X. Cao et al., Anion-anchored polymer-in-salt solid electrolyte for high-performance zinc batteries. Angew. Chem. Int. Ed. 64(2), e202414777 (2025). https://doi.org/10.1002/anie.202414777
  17. C. Dong, Y. Yu, C. Ma, C. Zhou, J. Wang et al., Tailoring zinc diatomic bidirectional catalysts achieving orbital coupling–hybridization for ultralong-cycling zinc–iodine batteries. Energy Environ. Sci. 18(6), 3014–3025 (2025). https://doi.org/10.1039/d4ee05767h
  18. W. Yan, Y. Liu, J. Qiu, F. Tan, J. Liang et al., A tripartite synergistic optimization strategy for zinc-iodine batteries. Nat. Commun. 15(1), 9702 (2024). https://doi.org/10.1038/s41467-024-53800-6
  19. X. Yang, M. Xie, Z. Yan, H. Ruan, C. Yang et al., High-iodine-loading quasi-solid-state zinc–iodine batteries enabled by a continuous ion-transport network. Energy Environ. Sci. 18(10), 4730–4739 (2025). https://doi.org/10.1039/D5EE01170A
  20. X. Zhang, Q. Tang, H. Luo, W. Xie, B. Wang et al., Multivariate competitive coordination structure in hydrated eutectic electrolytes for ultra-long low-temperature aqueous zinc-ion electrochemistry. Adv. Energy Mater. 16, e04638 (2026). https://doi.org/10.1002/aenm.202504638
  21. D. Zhang, Y. Yue, X. Rao, D. Zhang, W. Limphirat et al., Redox-guided hydration engineering of sodium vanadate for ultrastable aqueous zinc-ion storage. Nano Energy 145, 111450 (2025). https://doi.org/10.1016/j.nanoen.2025.111450
  22. Z. Li, Z. Wang, W. Sun, Y. Ma, W. Guo et al., Regulating interface engineering by Helmholtz plane reconstructed achieves highly reversible zinc metal anodes. Adv. Mater. 37(14), e2420489 (2025). https://doi.org/10.1002/adma.202420489
  23. H. Wu, W. Ma, L. Wu, W. Dong, Y. Li et al., Suppressing dendrite growth by dolosse-structured ZIF-67 polycrystalline membranes through eliminating interfacial electrolyte turbulence on zinc anode. Angew. Chem. Int. Ed. 64(25), e202506222 (2025). https://doi.org/10.1002/anie.202506222
  24. P. Liang, G. Zhu, W. Wang, C.-L. Huang, S.-C. Wu et al., Carbon nanotubes for rechargeable Na/Cl2 batteries. J. Am. Chem. Soc. 147(22), 18541–18549 (2025). https://doi.org/10.1021/jacs.4c18070
  25. M. Liu, K.K. Abdalla, M. Xu, X. Li, R. Wang, Q. Li, Y. Zhao, “Proton-iodine” regulation of protonated polyaniline catalyst for high-performance electrolytic Zn-I2 batteries. Nano-Micro Lett. 18(1), 1–14 (2026). https://doi.org/10.1007/s40820-025-01928-5
  26. D.Q. Cai, H. Xu, T. Xue, J.L. Yang, H.J. Fan, A synchronous strategy to Zn-iodine battery by polycationic long-chain molecules. Nano-Micro Lett. 18(1), 3 (2026). https://doi.org/10.1007/s40820-025-01854-6
  27. X. Luo, L. Jiao, D. Chao, F. Li, R. Wang et al., Synergistic effects of electrolyte additives in a dual-salt system for high-performance four electron aqueous zinc-iodine batteries across a wide temperature range. Angew. Chem. Int. Ed. 64(42), e202514375 (2025). https://doi.org/10.1002/anie.202514375
  28. T. Yan, B. Wu, S. Liu, M. Tao, J. Liang et al., Sieving-type electric double layer with hydrogen bond interlocking to stable zinc metal anode. Angew. Chem. Int. Ed. 63(47), e202411470 (2024). https://doi.org/10.1002/anie.202411470
  29. J. Cao, Y. Sun, Y. Jin, X. Rao, D. Luo et al., Molecular interface engineering enables hybrid SEI formation for long-cycle zinc metal anodes. Chem. Eng. J. 519, 165147 (2025). https://doi.org/10.1016/j.cej.2025.165147
  30. D. Zhang, J. Cao, C. Yang, K. Lolupiman, W. Limphirat et al., Highly stable aqueous Zn-ion batteries achieved by suppressing the active component loss in vanadium-based cathode. Adv. Energy Mater. 15(15), 2404026 (2025). https://doi.org/10.1002/aenm.202404026
  31. J. Cao, X. Wang, S. Qian, D. Zhang, D. Luo et al., De-passivation and surface crystal plane reconstruction via chemical polishing for highly reversible zinc anodes. Adv. Mater. 36(46), 2410947 (2024). https://doi.org/10.1002/adma.202410947
  32. P. Hei, Y. Sai, L. Yu, Y. Lin, B. Li et al., Cosolvent electrolyte design for high-voltage aqueous zinc-sulfur batteries. J. Am. Chem. Soc. 147(31), 27802–27811 (2025). https://doi.org/10.1021/jacs.5c06710
  33. Y. Lv, C. Huang, M. Zhao, M. Fang, Q. Dong et al., Synergistic anion-cation chemistry enables highly stable Zn metal anodes. J. Am. Chem. Soc. 147(10), 8523–8533 (2025). https://doi.org/10.1021/jacs.4c16932
  34. L. Liu, X. Wang, Z. Hu, X. Wang, Q. Zheng et al., Electric double layer regulator design through a functional group assembly strategy towards long-lasting zinc metal batteries. Angew. Chem. Int. Ed. 63(30), e202405209 (2024). https://doi.org/10.1002/anie.202405209
  35. Y. Meng, M. Wang, J. Wang, X. Huang, X. Zhou et al., Robust bilayer solid electrolyte interphase for Zn electrode with high utilization and efficiency. Nat. Commun. 15(1), 8431 (2024). https://doi.org/10.1038/s41467-024-52611-z
  36. J. Chen, G. Ou, P. Liu, W. Fan, B. Li et al., Pyrrolic-nitrogen chemistry in 1-(2-hydroxyethyl)imidazole electrolyte additives toward a 50, 000-cycle-life aqueous zinc-iodine battery. Angew. Chem. Int. Ed. 64(2), e202414166 (2025). https://doi.org/10.1002/anie.202414166
  37. Y. Wang, Y. Cui, M. Zhao, J. Wang, X. Liu et al., Zwitterion-mediated interface chemistry for practical Zn-iodine batteries. Nat. Commun. 16, 5565 (2025). https://doi.org/10.1038/s41467-025-60488-9
  38. X. Huang, T. Pan, B. Zhang, J. Wang, T. Hu et al., Functionally segregated ion regulation enables dual confinement effect for highly stable zinc-iodine batteries. Adv. Mater. 37(30), e2500500 (2025). https://doi.org/10.1002/adma.202500500
  39. T. Yang, T. Su, M. Xu, D. Wang, W. Ren et al., Dienoic-acid coupling effect induced hierarchical interface for high-performance zinc metal batteries. Angew. Chem. Int. Ed. 64(41), e202512780 (2025). https://doi.org/10.1002/anie.202512780
  40. H. Wu, S.-J. Zhang, J. Vongsvivut, M. Jaroniec, J. Hao et al., Aqueous zinc-iodine batteries with ultra-high loading and advanced performance. Joule 9(7), 102000 (2025). https://doi.org/10.1016/j.joule.2025.102000
  41. S.-J. Zhang, J. Hao, H. Wu, Q. Chen, C. Ye et al., Protein interfacial gelation toward shuttle-free and dendrite-free Zn-iodine batteries. Adv. Mater. 36(35), e2404011 (2024). https://doi.org/10.1002/adma.202404011
  42. C. Wu, Y. Pan, Y. Jiao, P. Wu, α-methyl group reinforced amphiphilic poly(ionic liquid) additive for high-performance zinc-iodine batteries. Angew. Chem. Int. Ed. 64(21), e202423326 (2025). https://doi.org/10.1002/anie.202423326
  43. J. Huang, Y. Zhong, N. AlMasoud, T.S. Alomar, Y. Xie et al., Tailored fluoroborate-based electrolyte with fast interphase formation kinetics toward stable Ah-level zinc batteries. Adv. Powder Mater. 4(4), 100306 (2025). https://doi.org/10.1016/j.apmate.2025.100306
  44. X. Hu, G. Lai, Y. Liu, P. Zhou, B. Lu et al., Design of dual-electrode interfacial kinetics regulator for long-lasting Ah-level zinc-iodine batteries. EScience 5(6), 100455 (2025). https://doi.org/10.1016/j.esci.2025.100455
Read More
Author biographies are not available.
Download this PDF file
PDF SUPPLEMENTARY FILE

Most read articles by the same author(s)