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Vol. 18 (2026)

Zincophilic–Hydrophobic Interface Design for Dendrite-Free Aqueous Zinc-Ion Batteries

https://doi.org/10.1007/s40820-026-02153-4
Yinfeng Guo
State Key Laboratory of Advanced Fiber Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, People’s Republic of China
Yuxiang Xu
State Key Laboratory of Advanced Fiber Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, People’s Republic of China
Yaduo Jia
Tianjin Key Laboratory of Materials Laminating Fabrication and Interface Control Technology, School of Materials Science and Engineering, Hebei University of Technology, Tianjin 300130, People’s Republic of China
Xiaoqing Zhu
State Key Laboratory of Advanced Fiber Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, People’s Republic of China
Tao Zhang
State Key Laboratory of Advanced Fiber Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, People’s Republic of China
Jia Zhang
State Key Laboratory of Advanced Fiber Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, People’s Republic of China
Changyong Chase Cao
Department of Mechanical and Aerospace Engineering, Case Western Reserve University, Cleveland, OH 44106, USA
Qilin Gu
NJTECH University Suzhou Future Membrane Technology Innovation Center, Suzhou 215100, People’s Republic of China
Guiyin Xu
State Key Laboratory of Advanced Fiber Materials, College of Materials Science and Engineering, Donghua University, Shanghai 201620, People’s Republic of China

Corresponding Author: Guiyin Xu

xuguiyin@dhu.edu.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 324

Abstract

Achieving Zn anode stability is critical for advancing commercialization of aqueous zinc-ion batteries. However, the instability of zinc metal anodes driven by dendritic growth, hydrogen evolution, and interfacial passivation remains a critical obstacle for advancing aqueous zinc-ion batteries. In this paper, we report a synergistic interfacial engineering strategy that integrates in situ-grown zincophilic copper nanorod arrays with a self-assembled layer of 1-dodecanethiol to regulate ion flux and suppress side reactions simultaneously. The water-poor electric double-layer microenvironment derived from this dual-function “zincophilic–hydrophobic” architecture (denoted as HS-Cu@Zn) promotes uniform Zn deposition along the (100) plane, enhances desolvation kinetics (Zn2+ transference number increased from 0.47 to 0.75), and effectively excludes electroactive water molecules from the anode surface. As a result, the symmetric cells exhibit ultra-long cycling stability over 3500 h at 1 mA cm−2, while Zn||Cu half-cells maintain a Coulombic efficiency of 99.65% for 900 cycles. ZnVO||HS-Cu@Zn full cell demonstrates exceptional cycling stability, achieving 2000 stable cycles at 5 A g−1 with an average Coulombic efficiency of 99.8%.


Highlights:
1 The loose rough surface of the Cu nanorod arrays provided ordered zinc migration channels and was used as a conductive substrate to modulate the nucleation sites of Zn2+, thereby promoting the uniform deposition of Zn2+.
2 The self-assembled layer of thiol molecules effectively reduces the concentration of water molecules at the interface of the Zn anode, ensuring the stability and reversibility of the Zn anode.
3 The synergistic interfacial engineering strategy reduced the desolvation energy of zinc ions and achieved a higher ion transfer number.

Keywords

Aqueous zinc-based batteries Zinc anode Interface regulation
Guo, Yinfeng, Yuxiang Xu, Yaduo Jia, Xiaoqing Zhu, Tao Zhang, Jia Zhang, Changyong Chase Cao, Qilin Gu, and Guiyin Xu. 2026. “Zincophilic–Hydrophobic Interface Design for Dendrite-Free Aqueous Zinc-Ion Batteries”. Nano-Micro Letters 18 (April):324. https://doi.org/10.1007/s40820-026-02153-4.
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References
  1. B. Tang, G. Fang, J. Zhou, L. Wang, Y. Lei et al., Potassium vanadates with stable structure and fast ion diffusion channel as cathode for rechargeable aqueous Zinc-ion batteries. Nano Energy 51, 579–587 (2018). https://doi.org/10.1016/j.nanoen.2018.07.014
  2. W. Zhang, Y. Dai, R. Chen, Z. Xu, J. Li et al., Highly reversible zinc metal anode in a dilute aqueous electrolyte enabled by a pH buffer additive. Angew. Chem. Int. Ed. 62(5), e202212695 (2023). https://doi.org/10.1002/anie.202212695
  3. X. Luo, T. Shen, C. Liu, Toward stable and safe Zinc metal anodes in aqueous rechargeable batteries. Adv. Sustain. Syst. 9(12), e01189 (2025). https://doi.org/10.1002/adsu.202501189
  4. F. Wang, O. Borodin, T. Gao, X. Fan, W. Sun et al., Highly reversible zinc metal anode for aqueous batteries. Nat. Mater. 17(6), 543–549 (2018). https://doi.org/10.1038/s41563-018-0063-z
  5. T. Shen, C. Li, Y. Wang, Z. Li, M. Yang et al., Fluorinated aromatic anode-electrolyte interface for highly reversible zinc anode. Adv. Funct. Mater. 35(47), 2509705 (2025). https://doi.org/10.1002/adfm.202509705
  6. M. Wang, J. Ma, Y. Meng, J. Sun, Y. Yuan et al., High-capacity zinc anode with 96% utilization rate enabled by solvation structure design. Angew. Chem. Int. Ed. 62(3), e202214966 (2023). https://doi.org/10.1002/anie.202214966
  7. F. Ming, Y. Zhu, G. Huang, A.-H. Emwas, H. Liang et al., Co-solvent electrolyte engineering for stable anode-free zinc metal batteries. J. Am. Chem. Soc. 144(16), 7160–7170 (2022). https://doi.org/10.1021/jacs.1c12764
  8. Z. Mai, Y. Lin, J. Sun, C. Wang, G. Yang et al., Breaking performance limits of zn anodes in aqueous batteries by tailoring anion and cation additives. Nano-Micro Lett. 17(1), 259 (2025). https://doi.org/10.1007/s40820-025-01773-6
  9. Y. Zong, H. He, Y. Wang, M. Wu, X. Ren et al., Functionalized separator strategies toward advanced aqueous zinc-ion batteries. Adv. Energy Mater. 13(20), 2300403 (2023). https://doi.org/10.1002/aenm.202300403
  10. Y. Li, X. Peng, X. Li, H. Duan, S. Xie et al., Functional ultrathin separators proactively stabilizing zinc anodes for zinc-based energy storage. Adv. Mater. 35(18), e2300019 (2023). https://doi.org/10.1002/adma.202300019
  11. T. Wang, P. Wang, L. Pan, Z. He, L. Dai et al., Stabling zinc metal anode with polydopamine regulation through dual effects of fast desolvation and ion confinement. Adv. Energy Mater. 13(5), 2203523 (2023). https://doi.org/10.1002/aenm.202203523
  12. X. Xie, S. Liang, J. Gao, S. Guo, J. Guo et al., Manipulating the ion-transfer kinetics and interface stability for high-performance zinc metal anodes. Energy Environ. Sci. 13(2), 503–510 (2020). https://doi.org/10.1039/C9EE03545A
  13. S.-B. Wang, Q. Ran, R.-Q. Yao, H. Shi, Z. Wen et al., Lamella-nanostructured eutectic zinc-aluminum alloys as reversible and dendrite-free anodes for aqueous rechargeable batteries. Nat. Commun. 11(1), 1634 (2020). https://doi.org/10.1038/s41467-020-15478-4
  14. L. Cao, D. Li, T. Pollard, T. Deng, B. Zhang et al., Fluorinated interphase enables reversible aqueous zinc battery chemistries. Nat. Nanotechnol. 16(8), 902–910 (2021). https://doi.org/10.1038/s41565-021-00905-4
  15. L. Kang, M. Cui, F. Jiang, Y. Gao, H. Luo et al., Nanoporous CaCO3 coatings enabled uniform Zn stripping/plating for long-life zinc rechargeable aqueous batteries. Adv. Energy Mater. 8(25), 1801090 (2018). https://doi.org/10.1002/aenm.201801090
  16. K. Wu, J. Yi, X. Liu, Y. Sun, J. Cui et al., Regulating Zn deposition via an artificial solid-electrolyte interface with aligned dipoles for long life Zn anode. Nano-Micro Lett. 13(1), 79 (2021). https://doi.org/10.1007/s40820-021-00599-2
  17. P. Chen, X. Yuan, Y. Xia, Y. Zhang, L. Fu et al., An artificial polyacrylonitrile coating layer confining zinc dendrite growth for highly reversible aqueous zinc-based batteries. Adv. Sci. 8(11), 2100309 (2021). https://doi.org/10.1002/advs.202100309
  18. L. Hong, L.-Y. Wang, Y. Wang, X. Wu, W. Huang et al., Toward hydrogen-free and dendrite-free aqueous zinc batteries: formation of zincophilic protective layer on Zn anodes. Adv. Sci. 9(6), 2104866 (2022). https://doi.org/10.1002/advs.202104866
  19. X. Zhou, B. Wen, Y. Cai, X. Chen, L. Li et al., Interfacial engineering for oriented crystal growth toward dendrite-free Zn anode for aqueous zinc metal battery. Angew. Chem. Int. Ed. 63(21), e202402342 (2024). https://doi.org/10.1002/anie.202402342
  20. P. Xiao, H. Li, J. Fu, C. Zeng, Y. Zhao et al., An anticorrosive zinc metal anode with ultra-long cycle life over one year. Energy Environ. Sci. 15(4), 1638–1646 (2022). https://doi.org/10.1039/D1EE03882F
  21. P. Ruan, X. Chen, L. Qin, Y. Tang, B. Lu et al., Achieving highly proton-resistant Zn-Pb anode through low hydrogen affinity and strong bonding for long-life electrolytic Zn//MnO2 battery. Adv. Mater. 35(31), e2300577 (2023). https://doi.org/10.1002/adma.202300577
  22. C. Liu, J. Zeng, S. Di, S. Wang, L. Li, An interfacial dual-regulation strategy for ultra-stable 3D Zn metal anodes. Acta Mater. 281, 120433 (2024). https://doi.org/10.1016/j.actamat.2024.120433
  23. Y. Xin, J. Qi, H. Xie, Y. Ge, Z. Wang et al., 3D ternary alloy artificial interphase toward ultra-stable and dendrite-free aqueous zinc batteries. Adv. Funct. Mater. 34(39), 2403222 (2024). https://doi.org/10.1002/adfm.202403222
  24. G. Zhang, X. Li, K. Chen, Y. Guo, D. Ma et al., Tandem electrocatalytic nitrate reduction to ammonia on MBenes. Angew. Chem. Int. Ed. 62(13), e202300054 (2023). https://doi.org/10.1002/anie.202300054
  25. J.C. Love, L.A. Estroff, J.K. Kriebel, R.G. Nuzzo, G.M. Whitesides, Self-assembled monolayers of thiolates on metals as a form of nanotechnology. ChemInform 36(32), 200532281 (2005). https://doi.org/10.1002/chin.200532281
  26. S. Wei, Z.-H. Qi, Y. Xia, S. Chen, C. Wang et al., Monolayer thiol engineered covalent interface toward stable zinc metal anode. ACS Nano 16(12), 21152–21162 (2022). https://doi.org/10.1021/acsnano.2c09111
  27. S. Han, M. Li, Q. Fan, Z. Han, X. Ming et al., Multifunctional additives with dynamic sacrificial S–S bonds for building self-assembled monolayers of Zn-ion batteries with improved stability and longevity. Energy Environ. Sci. 18(9), 4186–4199 (2025). https://doi.org/10.1039/d4ee05922k
  28. Z. Fan, W. Zhao, S. Shi, M. Zhou, J. Li et al., Regulating electric double layer via self-assembled monolayer for stable solid/electrolyte interphase on Mg metal anode. Angew. Chem. Int. Ed. 64(4), e202416582 (2025). https://doi.org/10.1002/anie.202416582
  29. W. Peng, L. Li, X. Bai, P. Yi, Y. Xie et al., Observation of ice-like two-dimensional flakes on self-assembled protein monolayer without nanoconfinement under ambient conditions. Nano-Micro Lett. 17(1), 187 (2025). https://doi.org/10.1007/s40820-025-01689-1
  30. Y. Liu, D. Ji, W. Hu, Recent progress of interface self-assembled monolayers engineering organic optoelectronic devices. DeCarbon 3, 100035 (2024). https://doi.org/10.1016/j.decarb.2024.100035
  31. F. Xu, Y. Tang, H. Wang, H. Deng, Y. Huang et al., Using wool keratin derived metallo-nanozymes as a robust antioxidant catalyst to scavenge reactive oxygen species generated by smoking. Small 18(23), 2201205 (2022). https://doi.org/10.1002/smll.202201205
  32. J. Lu, J. Wang, Q. Zou, D. He, L. Zhang et al., Unravelling the nature of the active species as well as the doping effect over Cu/Ce-based catalyst for carbon monoxide preferential oxidation. ACS Catal. 9(3), 2177–2195 (2019). https://doi.org/10.1021/acscatal.8b04035
  33. J. Liu, S. Duan, A. Chen, X. Liu, C. Tian et al., Unveiling the valid active site of copper nano-electrocatalysts by surface reconstruction for enhanced nitrate reduction to ammonia. J. Energy Chem. 116, 339–346 (2026). https://doi.org/10.1016/j.jechem.2026.01.001
  34. X. Bu, J. Li, J. Wang, Y. Li, G. Zhang, Boosting charge transfer promotes photocatalytic peroxymonosulfate activation of S-doped CuBi2O4 nanorods for ciprofloxacin degradation: key role of Ov–Cu–S and mechanism insight. Chem. Eng. J. 494, 153075 (2024). https://doi.org/10.1016/j.cej.2024.153075
  35. H. Yu, D. Chen, Q. Li, C. Yan, Z. Jiang et al., In situ construction of anode–molecule interface via lone-pair electrons in trace organic molecules additives to achieve stable zinc metal anodes. Adv. Energy Mater. 13(22), 2300550 (2023). https://doi.org/10.1002/aenm.202300550
  36. T. Wu, C. Hu, Q. Zhang, Z. Yang, G. Jin et al., Helmholtz plane reconfiguration enables robust zinc metal anode in aqueous zinc-ion batteries. Adv. Funct. Mater. 34(30), 2315716 (2024). https://doi.org/10.1002/adfm.202315716
  37. L. Wang, Y. Shao, Z. Fu, X. Zhang, J. Kang et al., Synergistically enhancing the selective adsorption for crystal planes to regulate the (002)-texture preferred Zn deposition via supramolecular host–guest units. Energy Environ. Sci. 18(10), 4859–4871 (2025). https://doi.org/10.1039/d5ee00763a
  38. J. Feng, X. Li, Y. Ouyang, H. Zhao, N. Li et al., Regulating Zn2+ migration-diffusion behavior by spontaneous cascade optimization strategy for long-life and low N/P ratio zinc ion batteries. Angew. Chem. Int. Ed. 63(41), e202407194 (2024). https://doi.org/10.1002/anie.202407194
  39. Z. Peng, S. Li, L. Tang, J. Zheng, L. Tan et al., Water-shielding electric double layer and stable interphase engineering for durable aqueous zinc-ion batteries. Nat. Commun. 16(1), 4490 (2025). https://doi.org/10.1038/s41467-025-59830-y
  40. X. Zhao, M. Yan, J. Bi, K. Kong, L. Liu et al., Unveiling electrode–electrolyte interface dynamics for aqueous Zn batteries. ACS Energy Lett. 10(5), 2400–2409 (2025). https://doi.org/10.1021/acsenergylett.5c00445
  41. J. Liu, C. Li, Q. Lv, D. Chen, J. Zhao et al., Reconstruction of electric double layer on the anode interface by localized electronic structure engineering for aqueous Zn ion batteries. Adv. Energy Mater. 14(29), 2401118 (2024). https://doi.org/10.1002/aenm.202401118
  42. C. Yan, F. He, L. Feng, L. Zhu, P. Li et al., Interfacial molecule engineering builds tri-functional bilayer silane films with hydrophobic ion channels for highly stable Zn metal anode. Adv. Funct. Mater. 35(35), 2503493 (2025). https://doi.org/10.1002/adfm.202503493
  43. Y. Aniskevich, S.-T. Myung, Gains and losses in zinc-ion batteries by proton- and water-assisted reactions. Chem. Soc. Rev. 54(9), 4531–4566 (2025). https://doi.org/10.1039/D4CS00810C
  44. Z. Wang, X. Zhu, X. Tao, P. Feng, J. Wang et al., Realizing high reversible zinc metal anode by modulating surface chemistry and crystal structure. Adv. Funct. Mater. 34(26), 2316223 (2024). https://doi.org/10.1002/adfm.202316223
  45. H. Yang, J. Wang, P. Zhang, X. Cheng, Q. Guan et al., Dielectric-ion-conductive ZnNb2O6 layer enabling rapid desolvation and diffusion for dendrite-free Zn metal batteries. J. Energy Chem. 100, 693–701 (2025). https://doi.org/10.1016/j.jechem.2024.09.010
  46. D. Wang, N. Zhang, Y. Zhang, L. Chang, H. Tang et al., Electric field sponge effect of conducting polymer interphases boosts the kinetics and stability of zinc metal anodes. Adv. Energy Mater. 15(11), 2404090 (2025). https://doi.org/10.1002/aenm.202404090
  47. W. Fan, C. Zhu, X. Wang, H. Wang, Y. Zhu et al., All-natural charge gradient interface for sustainable seawater zinc batteries. Nat. Commun. 16(1), 1273 (2025). https://doi.org/10.1038/s41467-025-56519-0
  48. L. Xiao, C. Yuan, P. Chen, Y. Liu, J. Sheng et al., Cu–S bonds as an atomic-level transfer channel to achieve photocatalytic CO2 reduction to CO on Cu-substituted ZnIn2S4. ACS Sustain. Chem. Eng. 10(36), 11902–11912 (2022). https://doi.org/10.1021/acssuschemeng.2c02919
  49. J. Cao, Y. Jin, H. Wu, Y. Yue, D. Zhang et al., Enhancing zinc anode stability with gallium ion-induced electrostatic shielding and oriented plating. Adv. Energy Mater. 15(6), 2403175 (2025). https://doi.org/10.1002/aenm.202403175
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