Turn off MathJax
Article Contents
Article Navigation >  Green Energy&Environment  > 2026  > Accepted Manuscript
Wenzhen Du, Ju Liu, Yue Zhu, Shenglong Wu, Yaqin Wang, Shaojie Feng, Junwu Chen, Qiongguang Li, Hongyan He. Disrupting Interfacial Hydrogen-Bond Networks to Build a Local H2O-Poor Microenvironment for Durable Aqueous Zn Anodes. Green Energy&Environment. doi: 10.1016/j.gee.2026.06.006
Citation: Wenzhen Du, Ju Liu, Yue Zhu, Shenglong Wu, Yaqin Wang, Shaojie Feng, Junwu Chen, Qiongguang Li, Hongyan He. Disrupting Interfacial Hydrogen-Bond Networks to Build a Local H2O-Poor Microenvironment for Durable Aqueous Zn Anodes. Green Energy&Environment. doi: 10.1016/j.gee.2026.06.006
shu

Disrupting Interfacial Hydrogen-Bond Networks to Build a Local H2O-Poor Microenvironment for Durable Aqueous Zn Anodes

doi: 10.1016/j.gee.2026.06.006

  • a. Anhui Province International Research Center on Advanced Building Materials, School of Materials and Chemical Engineering, Anhui Jianzhu University, Hefei 230601, China;

  • b. Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Normal University, Wuhu 230061, China;

  • c. Beijing Key Laboratory of Solid State Battery and Energy Storage Process, State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;

  • d. Laboratory of Artificial Chemical Intelligence (LIAC), Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne 1015, Switzerland;

  • e. Anhui Institute of Strategic Study on Carbon Dioxide Emissions Peak and Carbon Neutrality in Urban-Rural Development, Anhui Jianzhu University, Hefei 230601, China;

  • f. University of Chinese Academy of Sciences, Beijing 100049, China

Funds:

This work was financially supported by the Doctoral Scientific Research Startup Foundation of Anhui Jianzhu University (Grant No. 2022QDZ01), the Open Project Program of Key Laboratory of Functional Molecular Solids of Ministry of Education (FMS2023004), Anhui Province International Research Center on Advanced Building Materials (Grant No. JZCL2303ZR) and Anhui Institute of Strategic Study on Carbon Dioxide Emissions Peak and Carbon Neutrality in Urban-Rural Development (Grant No. STY-2023-05).

  • Received date 06 February 2026, Accepted date 10 June 2026, RevRecd date 13 April 2026, Available online 22 June 2026
    Abstract
  • Aqueous zinc metal anodes (ZMAs) suffer from H2O-driven parasitic reactions and dendritic plating, both rooted at the electrode-electrolyte interface. Herein, we report a molecular microenvironment engineering strategy that disrupts the interfacial hydrogen-bond (HB) network dynamically to deplete interfacial H2O at the ZMA surface. The low-molecular-weight additive N-methylsuccinimide (NMS) exhibits stronger HB interactions with H2O and high affinity for Zn than H2O itself, thereby displacing interfacial H2O and enriching the Helmholtz double layer with NMS. Together with its fast self-diffusion and robust Zn2+ coordination capability, NMS accelerates Zn2+ transport, effectively compensating for the interfacial Zn2+ consumption and alleviating local concentration polarization. Consequently, ZMAs achieve dense, highly ordered Zn deposits with a preferential (101) orientation, while parasitic reactions are markedly suppressed. As a result, ZnZn symmetric cells cycle for >1730 h at 10 mA cm-2 and 1 mAh cm-2 without short circuiting, and ZnV2O5 full cells sustain reliable operation for >2500 cycles at 10 A g-1. Combined MD/DFT calculations and in situ/operando characterizations support a dynamic solvation-displacement mechanism that reconstructs the interfacial HB network. Beyond enhanced performance, this interfacial HB-network regulation provides a generalizable paradigm for controlling solvation–reaction coupling in aqueous metal batteries.

     

    • FullText(HTML)
  • loading
    • References(57)
  • [1]
    Y. Geng, L. Pan, Z. Peng, Z. Sun, H. Lin, C. Mao, L. Wang, L. Dai, H. Liu, K. Pan, X. Wu, Q. Zhang, Z. He, Energy Storage Mater. 51 (2022) 733-755.
    [2]
    C. Nie, G. Wang, D. Wang, M. Wang, X. Gao, Z. Bai, N. Wang, J. Yang, Z. Xing, S. Dou, Adv. Energy Mater. 13 (2023) 2300606.
    [3]
    Z. Yi, G. Chen, F. Hou, L. Wang, J. Liang, Adv. Energy Mater. 11 (2020) 2300606.
    [4]
    H. Lin, L. Zeng, C. Lin, J. Wu, H. He, C. Huang, W. Lai, P. Xiong, F. Xiao, Q. Qian, Q. Chen, J. Lu, Energy Environ. Sci. 18 (2025) 1282-1293.
    [5]
    X. Wang, W. Zhou, L. Wang, Y. Zhang, S. Li, X. Li, Z. Zhao, T. Zhang, H. Jin, X. Song, P. Liang, B. Zhang, D. Zhao, D. Chao, Adv. Mater. 37 (2025) 2501049.
    [6]
    D. Li, Y. Guo, C. Zhang, X. Chen, W. Zhang, S. Mei, C.J. Yao, Nano-Micro Lett. 16 (2024) 194.
    [7]
    G. Jiang, R. Xue, L. He, J. Zhu, N. Qiu, Y. Wang, Chem. Eng. J. 472 (2023) 145016.
    [8]
    J. Zhu, X. Ge, Z. Peng, L. Pan, Z. Peng, Y. Jiang, W. Meng, Z. Zhang, N. Zhao, B. Li, L. Dai, L. Wang, Z. He, Green Energy Environ. 10 (2025) 689-708.
    [9]
    L. Xie, Y. Zhu, Y. Du, Y. Yang, H. Chen, Z. Wang, G. Huang, B. Zhang, Green Energy Environ. 10 (2025) 1559-1567.
    [10]
    Z. Teng, Y. Luo, S. Su, W. Miao, C. Zhang, L. Wu, W. Chen, Chem. Eng. J. 515 (2025) 163454.
    [11]
    J. Zhang, Y. Wang, Z. Zhao, P. Li, G. Tang, W. Chen, Z. Peng, Adv. Energy Mater. 14 (2024) 2401560.
    [12]
    M. Shi, C. Lei, H. Wang, P. Jiang, C. Xu, W. Yang, X. He, X. Liang, Angew. Chem. Int. Ed. 63 (2024) 202407261.
    [13]
    W. Du, C. Wang, Y. Zhu, S. Wu, W. Liu, Y. Wang, S. Feng, M. Yao, Y. Huang, Q. Li, Chem. Eng. J. 515 (2025) 163642.
    [14]
    H. Yang, K. Zhu, W. Xie, W. Yang, ACS Nano 19 (2025) 1433-1446.
    [15]
    C. Huang, X. Zhao, S. Liu, Y. Hao, Q. Tang, A. Hu, Z. Liu, X. Chen, Adv. Mater. 33 (2021).
    [16]
    Q. Kang, H. Liang, Z. Zhu, F. Xing, B. Zhu, Y. Li, S. Wang, S. Tang, H. Li, L. Pan, L. Yang, T. Mo, Y. Bu, Angew. Chem. Int. Ed. 64 (2025) 202420183.
    [17]
    C. Liu, W.B. Jiang, D. Xie, W.Y. Diao, F.Y. Tao, X.Z. Wang, H.Z. Sun, W.L. Li, X.L. Wu, J.P. Zhang, Small 19 (2023) 2304751.
    [18]
    R. Sun, D. Han, C. Cui, Z. Han, X. Guo, B. Zhang, Y. Guo, Y. Liu, Z. Weng, Q.H. Yang, Angew. Chem. Int. Ed. 62 (2023) 202303557.
    [19]
    X. Yang, X. Nie, C. Tang, Y. Xiao, Q. Li, D. Yuan, M. Yao, Nano Res. 18 (2025) 94907031.
    [20]
    Z. Liu, S. Chen, Z. Shi, P. Qiu, K. He, Q. Lu, M. Yu, T. Liu, Adv. Energy Mater. 15 (2025) 2502010.
    [21]
    Y. Li, H. Wang, T. Wu, C. Xie, Z. Yang, Q. Zhang, D. Sun, Y. Tang, L. Fu, H. Wang, Sci. China Chem. 66 (2023) 1844-1853.
    [22]
    G.C. Gschwend, H.H. Girault, Chem. Sci. 11 (2020) 10304-10312.
    [23]
    R. Sivkova, J. Svoboda, J. Panek, D. Appelhans, O. Pop-Georgievski, Prog. Org. Coat. 178 (2023) 107447.
    [24]
    Y. Yang, Y. Li, Q. Zhu, B. Xu, Adv. Funct. Mater. 34 (2024) 2316371.
    [25]
    T. Li, C. Lin, M. Luo, P. Wang, D. Li, S. Li, J. Zhou, H. Yang, ACS Energy Lett. 8 (2023) 3258-3268.
    [26]
    P. Sun, Y.Q. Zheng, X. Zhang, H. Yu, Y. Guo, L. Yu, Adv. Energy Mater. 14 (2024) 2304138.
    [27]
    S. Li, J. Zhao, X. Xu, J. Shen, K. Zhang, X. Chen, K. Wang, X. Jiao, Z. Wang, D. Xu, Q. Zhang, Y. Liu, Y. Bai, Mater. Today 80 (2024) 50-60.
    [28]
    J. Cong, Z. Hu, L. Hu, T. Li, H. Ji, Z. Long, Y. Fan, Z. Wen, Y.C. Lin, H. Xu, Z. Li, S. Li, F. Pan, Y. Huang, Adv. Funct. Mater. 35 (2025) 2424423.
    [29]
    C. Li, X. Chang, B. Yuan, Y. Wang, X. Feng, C. Gu, K. Chen, Q. Meng, Y. Guo, L. Wan, J. Am. Chem. Soc. 147 (2025) 40925-40934.
    [30]
    P. Song, S. Guerin, S. Tan, H.V. Annadata, X. Yu, M. Scully, Y. Han, M. Roemer, K.P. Loh, D. Thompson, C.A. Nijhuis, Adv. Mater. 30 (2018) 1706322.
    [31]
    Y. Su, J. Hu, G. Yuan, G. Zhang, W. Wei, Y. Sun, X. Zhang, Z. Liu, N.T. Suen, H.C. Chen, H. Pang, Adv. Mater. 35 (2023) e2307003.
    [32]
    Q. Zhao, W. Liu, X. Ni, H. Yu, C. Zhang, B. Wang, L. Jiang, H. He, Y. Chen, L. Chen, Adv. Funct. Mater. 34 (2024) 2404219.
    [33]
    T. Sun, Q. Nian, X. Ren, Z. Tao, Joule 7 (2023) 2700-2731.
    [34]
    T. Ruan, J. Xu, X. Zhou, Z. Chen, J. Zhou, S. Lu, R. Li, J. Energy Chem. 110 (2025) 693-702.
    [35]
    T. Wu, C. Hu, Q. Zhang, Z. Yang, G. Jin, Y. Li, Y. Tang, H. Li, H. Wang, Adv. Funct. Mater. 34 (2024) 2315716.
    [36]
    T. Wu, C. Hu, Q. Zhang, Z. Yang, G. Jin, Y. Li, Y. Tang, H. Li, H. Wang, Adv. Funct. Mater. 34 (2024) 2315716.
    [37]
    Q. Zhang, J. Luan, X. Huang, Q. Wang, D. Sun, Y. Tang, X. Ji, H. Wang, Nat. Commun. 11 (2020) 3961.
    [38]
    Q. Li, C. Wang, W. Du, Y. Zhu, M. Yao, Y. Wang, S. Feng, R. Chen, J. Power Sources 625 (2025) 235673.
    [39]
    J. Li, S. Zhang, X. Yu, J. Li, H. Gu, Y. Long, N. Li, J. Han, Z. Yang, Nano Energy 141 (2025) 111049.
    [40]
    J. Chen, E. Quattrocchi, F. Ciucci, Y. Chen, Chem 9 (2023) 2267-2281.
    [41]
    R. Luo, X. Zheng, T. Jiang, D. Shen, M. Wang, M. Ali, H. Liu, Z. Zhang, Y. Feng, S. Hazoor, P. Tong, W. Chen, Adv. Energy Mater. 15 (2025) 202501658.
    [42]
    L. Wang, B. Zhang, W. Zhou, Z. Zhao, X. Liu, R. Zhao, Z. Sun, H. Li, X. Wang, T. Zhang, H. Jin, W. Li, A. Elzatahry, Y. Hassan, H.J. Fan, D. Zhao, D. Chao, J. Am. Chem. Soc. 146 (2024) 6199-6208.
    [43]
    S. Li, Y. Zhong, J. Huang, G. Lai, L. Li, L. Jiang, X. Xu, B. Lu, Y. Liu, J. Zhou, Energy Environ. Sci. 18 (2025) 2599-2609.
    [44]
    M. Yan, C. Xu, Y. Sun, H. Pan, H. Li, Nano Energy 82 (2021) 105739.
    [45]
    G. Guo, C. Ji, J. Lin, T. Wu, Y. Luo, C. Sun, M. Li, H. Mi, L. Sun, H.J. Seifert, Angew. Chem. Int. Ed. 63 (2024) 202407417.
    [46]
    H. Cao, X. Zhang, B. Xie, X. Huang, F. Xie, Y. Huo, Q. Zheng, R. Zhao, Q. Hu, L. Kang, S. Liu, D. Lin, Adv. Funct. Mater. 33 (2023) 202305683.
    [47]
    Q. Ren, X. Tang, Y. Guo, X. Liao, C. Zhang, Z. Zhu, P. Wang, W. Wang, Y. Li, W. Song, S. Wang, K. He, Z.B. Wang, Y. Yuan, Adv. Energy Mater. 15 (2024) 202403961.
    [48]
    L. Ren, Y. Dong, D. Zhong, Z. Su, A. Wang, C. Peng, J. Luo, Green Energy Environ. 10 (2025) 1819-1827.
    [49]
    L. Wang, F. Wang, Z. Ding, Y. Liu, Z. Zhang, C. Yang, K.P. Loh, Q. Yang, Green Energy Environ. 9 (2024) 771-776.
    [50]
    Y. Wang, Y. Cui, M. Zhao, J. Wang, X. Liu, Y. Zhu, Y. Yang, Nat. Commun. 16 (2025) 5565.
    [51]
    L. Wu, H. Yuan, Y. An, J. Sun, Y. Liu, H. Tang, W. Yang, L. Cui, J. Li, Q. An, Y. Zhang, L. Xu, L. Mai, Angew. Chem. Int. Ed. 64 (2024) 202419495.
    [52]
    J. Song, Z. Ren, Z. Chen, S. Zhang, Z. Yu, J. Cheng, B. Wang, Energy Storage Mater. 81 (2025) 104523.
    [53]
    N. Yu, S. Lin, S. Zhou, Y. Li, J. Li, Q. Zeng, L. Chen, L. Wang, K. Guo, X. Wang, Y. Li, Energy Storage Mater. 80 (2025) 104398.
    [54]
    Y. Chen, Z. Deng, Y. Sun, Y. Li, H. Zhang, G. Li, H. Zeng, X. Wang, Nano-Micro Lett. 16 (2024) 2-15.
    [55]
    F. Tao, Y. Ren, L.E. Mo, Y. Wang, Y. Huang, H. Zhang, C. Shi, Z. Li, J. Liu, L. Chen, L. Hu, Y. Wu, Nano-Micro Lett. 18 (2026) 107.
    [56]
    X. Xu, L. Su, X. Zhang, L. He, J. Li, F. Lu, L. Zheng, X. Gao, ACS Nano 20 (2026) 7158-7169.
    [57]
    G. Liang, Z. Gan, X. Wang, X. Jin, B. Xiong, X. Zhang, S. Chen, Y. Wang, H. He, C. Zhi, ACS Nano 15 (2021) 17717-17728.
    • Relative Articles
    • Supplements(0)
    • Cited By
  • 加载中

Catalog

    通讯作者: 陈斌, bchen63@163.com
    • 1. 

      沈阳化工大学材料科学与工程学院 沈阳 110142

    1. 本站搜索
    2. 百度学术搜索
    3. 万方数据库搜索
    4. CNKI搜索
    Get Citation
    PDF
    XML

    Article Metrics

    Article views (2) PDF downloads(0) Cited by()
    Proportional views

    Publish With GEE

    Contact

    • Email：gee@ipe.ac.cn
    • Tel：010-82627075
    • Address：North 2nd street, Zhongguancun, Haidian District, Beijing, China

    Links

    京ICP备10002620号-1京公网安备 11010802039050号

    Supported by: Beijing Renhe Information Technology Co. Ltd    

    /

    DownLoad:  Full-Size Img  PowerPoint
    Return
    Return