Citation: Wen Liu, Qiwen Zhao, Hongli Qi, Dongping Chen, Fengcheng Tang, Xiaoyu Liu, Huaming Yu, Gang Zhou, Yuejiao Chen, Libao Chen. Synergy of constructing robust hybrid interphase and weakly solvating electrolyte for low-temperature aqueous zinc-ion batteries[J]. Chinese Chemical Letters, ;2026, 37(5): 110893. doi: 10.1016/j.cclet.2025.110893 shu

Synergy of constructing robust hybrid interphase and weakly solvating electrolyte for low-temperature aqueous zinc-ion batteries

Wen Liu ^{a, b} ,
Qiwen Zhao ^b ,
Hongli Qi ^c ,
Dongping Chen ^c ,
Fengcheng Tang ^b ,
Xiaoyu Liu ^b ,
Huaming Yu ^{a, *,} ,
Gang Zhou ^{a, *,} ,
Yuejiao Chen ^b ,
Libao Chen ^b

a.
School of Materials Science and Engineering, Dongguan University of Technology, Dongguan 523808, China
b.
State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, China
c.
School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China

hmYu147@outlook.com

zhougang1986@dgut.edu.cn

Received Date: 9 December 2024
Revised Date: 14 January 2025
Accepted Date: 20 January 2025
Available Online: 21 January 2025

Figures(5)

Aqueous zinc-ion batteries (AZIBs) have emerged as strong contenders for large-scale energy storage solutions, attributed to their cost-effectiveness and enhanced safety profiles. Nevertheless, their widespread adoption is currently hindered by their poor performance in low-temperature conditions. Herein, an electrolyte is developed by utilizing weakly solvated and film-forming molecule dimethyl sulfite (DMS) to achieve smooth de-solvation and high ionic conductivity at low temperature. The DMS disrupts the hydrogen bonding network of water and lowers the freezing point of the electrolyte to -40.9 ℃. The designed electrolyte achieves ionic conductivity up to 10.75 mS/cm at -30 ℃. Due to the chemical reactivity of DMS and trifluoromethanesulfonate anions in the Zn²⁺-solvation shell, a ZnF₂-ZnS hybrid solid electrolyte interphase (SEI) is successively generated on Zn metal surface. Mechanistic studies reveal that such robust hybrid interphase can promote Zn²⁺ desolvation and rapid Zn²⁺ transport. In addition, the addition of DMS effectively suppresses the dendritic growth, hydrogen evolution reaction (HER), and corrosion-induced passivation on the anode surface, facilitating long-term cycling at subzero temperatures. At -40 ℃, the Zn//Zn symmetrical cell cycles for 1200 h at 0.5 mA/cm² and 0.5 mAh/cm², and the Zn//NVO cell achieves an ultra-long cycle life of 1000 cycles with a high capacity retention of 82.89% at 1 A/g.
- Weakly solvating electrolyte,
- Low-temperature batteries,
- Aqueous zinc-ion batteries,
- Low polarity co-solvent,
- Zn anode
1. [1]
  S. Huang, K. Li, Z. He, et al., J. Alloy. Compd. 1005 (2024) 176193. doi: 10.1016/j.jallcom.2024.176193
2. [2]
  Y. Zhong, C. Cao, L. Zhao, M.O. Tadé, Z. Shao, Green Carbon 2 (2024) 94–100. doi: 10.1016/j.greenca.2024.02.005
3. [3]
  D. Sun, Z. Sun, D. Yang, et al., EcoEnergy 1 (2023) 375–404. doi: 10.1002/ece2.22
4. [4]
  H.M. Yu, C.D. Lv, C.S. Yan, G.H. Yu, Small Methods 8 (2024) 2300758. doi: 10.1002/smtd.202300758
5. [5]
  W.D. Zhang, C. Sun, Y.X. Zhu, F. Gao, C. Lai, Rare Met. 43 (2024) 3044–3054. doi: 10.1007/s12598-024-02673-1
6. [6]
  F. Chen, Z.L. Xu, Microstructures 2 (2022) 2022012.
7. [7]
  J. Ren, H.Y. Wu, W. Yan, P. Huang, C. Lai, Ind. Chem. Mater. 2 (2024) 328–339. doi: 10.1039/D3IM00111C
8. [8]
  H. Yang, H.F. Zheng, H.M. Yu, et al., Nanoscale 14 (2022) 13722–13730. doi: 10.1039/D2NR04158H
9. [9]
  H. Yu, Z. He, D. Chen, et al., Energy Rev. 4 (2025) 100107. doi: 10.1016/j.enrev.2024.100107
10. [10]
  G. Ma, W. Yuan, X. Li, et al., Adv. Mater. 36 (2024) 2408287. doi: 10.1002/adma.202408287
11. [11]
  W. Qu, C. Wen, B. Chen, Y. Cai, M. Zhang, Sci. China Mater. 67 (2024) 2889–2897. doi: 10.1007/s40843-024-2971-y
12. [12]
  D. Tang, X. Zhang, D. Han, et al., Adv. Mater. 36 (2024) 2406071. doi: 10.1002/adma.202406071
13. [13]
  M. Cheng, D. Li, J. Cao, et al., Angew. Chem. Int. Ed. 63 (2024) e202410210.
14. [14]
  M. Qiu, Y. Liang, J. Hong, et al., Angew. Chem. Int. Ed. 63 (2024) e202407012. doi: 10.1002/anie.202407012
15. [15]
  X. Shi, J. Zeng, A. Yi, et al., J. Am. Chem. Soc. 146 (2024) 20508–20517. doi: 10.1021/jacs.4c07015
16. [16]
  J. Zhou, H. Yu, P. Qing, et al., J. Colloid Interface Sci. 678 (2025) 772–782. doi: 10.1016/j.jcis.2024.09.051
17. [17]
  C. Li, X. Jiang, H. Qi, et al., Energy Storage Mater. 75 (2025) 104012. doi: 10.1016/j.ensm.2025.104012
18. [18]
  S. Huang, R. Tang, X.Q. Liu, et al., Energy Environ. Sci. 17 (2024) 591–601. doi: 10.1039/D3EE02945J
19. [19]
  G.M. Qu, H. Wei, S.S. Zhao, et al., Adv. Mater. 36 (2024) 2400370. doi: 10.1002/adma.202400370
20. [20]
  W. Song, X. Xie, L. Deng, et al., Energy Storage Mater. 70 (2024) 103489. doi: 10.1016/j.ensm.2024.103489
21. [21]
  X. Guo, G. He, J. Mater. Chem. A 11 (2023) 11987–12001. doi: 10.1039/D3TA01904G
22. [22]
  R.Z. Zhao, X.S. Dong, P. Liang, et al., Adv. Mater. 35 (2023) 2209288. doi: 10.1002/adma.202209288
23. [23]
  X.P. Ma, H.M. Yu, C.S. Yan, et al., J. Colloid Interface Sci. 664 (2024) 539–548. doi: 10.1016/j.jcis.2024.03.085
24. [24]
  W. Kong, F. Wan, Y. Lei, et al., Anal. Chem. 96 (2024) 15313–15321.
25. [25]
  S.Z. Deng, B.G. Xu, J.X. Zhao, H. Fu, Energy Storage Mater. 70 (2024) 103490. doi: 10.1016/j.ensm.2024.103490
26. [26]
  D.D. Wang, H.L. Peng, S.J. Zhang, et al., Angew. Chem. Int. Ed. 62 (2023) e202315834. doi: 10.1002/anie.202315834
27. [27]
  M. Liu, L. Yao, Y. Ji, et al., Nano Lett. 23 (2023) 541–549. doi: 10.1021/acs.nanolett.2c03919
28. [28]
  Y.X. Zhao, S. Guo, M.J. Chen, et al., Nat. Commun. 14 (2023) 7080. doi: 10.1038/s41467-023-42919-7
29. [29]
  C. Zhang, C. Li, D. Chen, et al., J. Colloid Interface Sci. 682 (2025) 232–241. doi: 10.1016/j.jcis.2024.11.215
30. [30]
  Y.S. Li, X.D. Yang, Y. He, et al., Adv. Funct. Mater. 34 (2024) 2307736. doi: 10.1002/adfm.202307736
31. [31]
  S. Zhou, X. Meng, Y. Chen, et al., Angew. Chem. Int. Ed. 63 (2024) e202403050. doi: 10.1002/anie.202403050
32. [32]
  L. Wang, H. Yu, D. Chen, et al., Carbon Neutrality 3 (2024) 996–1008. doi: 10.1002/cnl2.168
33. [33]
  L.S. Han, Y.M. Guo, F.H. Ning, et al., Adv. Mater. 36 (2024) 2308086. doi: 10.1002/adma.202308086
34. [34]
  W. Wang, S. Chen, X. Liao, et al., Nat. Commun. 14 (2023) 5443. doi: 10.1038/s41467-023-41276-9
35. [35]
  Z. He, H. Yu, M. Fu, et al., Energy Storage Mater. 70 (2024) 103469. doi: 10.1016/j.ensm.2024.103469
36. [36]
  F. Bu, Y. Gao, W.B. Zhao, et al., Angew. Chem. Int. Ed. 63 (2024) e202318496. doi: 10.1002/anie.202318496
37. [37]
  N. Hu, W.S. Lv, W.J. Chen, et al., Adv. Funct. Mater. 34 (2024) 2311773. doi: 10.1002/adfm.202311773
38. [38]
  Y. Liu, H. Fu, C. Gao, et al., Adv. Energy Mater. 15 (2025) 2403562. doi: 10.1002/aenm.202403562
39. [39]
  H. Yu, D. Chen, L. Zhang, et al., Trans. Nonferrous Met. Soc. China 34 (2024) 3118–3150. doi: 10.1016/S1003-6326(24)66598-2
40. [40]
  Y. Bai, D. Deng, J. Wang, et al., Adv. Mater. 36 (2024) 2411404. doi: 10.1002/adma.202411404
41. [41]
  Q. Zhao, W. Liu, X. Ni, et al., Adv. Funct. Mater. 34 (2024) 2404219. doi: 10.1002/adfm.202404219
42. [42]
  C. Li, T. Liao, D. Chen, et al., Chin. Chem. Lett. 36 (2025) 110557. doi: 10.1016/j.cclet.2024.110557
43. [43]
  M.Y. Liu, W.T. Yuan, G.Q. Ma, et al., Angew. Chem. Int. Ed. 62 (2023) e202304444. doi: 10.1002/anie.202304444
1. [1]
  Haining Peng , Huijun Liu , Chengzong Li , Yingfu Li , Qizhi Chen , Tao Li . Diluent modified weakly solvating electrolyte for fast-charging high-voltage lithium metal batteries. Chinese Chemical Letters, 2025, 36(1): 109556-. doi: 10.1016/j.cclet.2024.109556
2. [2]
  Guangbin Wang , Binrui Xu , Bo Zhao , Yifei Pei , Haoming Li , Wanhong Zhang , Yong Liu . Alkaline lysine additive enables highly stable Zn anode for aqueous zinc-ion batteries. Chinese Chemical Letters, 2026, 37(5): 110859-. doi: 10.1016/j.cclet.2025.110859
3. [3]
  Sida Zhang , Huaping Mei , Baoyu Li , Feilin Yu , Kaxin Wang , Ruduan Yuan , Ziga Luogu , Zhixian Zhang , Xiqian Hu , Jianxin Wang , Xuetao Duan , Pinyi Wang , Wanlong Wu , Qianzhi Gou , Meng Li , Weigen Chen . Modulating the solvation sheath via bio-inspired electrolyte additives towards dendrite-free aqueous zinc ion batteries. Chinese Chemical Letters, 2026, 37(4): 111174-. doi: 10.1016/j.cclet.2025.111174
4. [4]
  Jun Guo , Zhenbang Zhuang , Wanqiang Liu , Gang Huang . "Co-coordination force" assisted rigid-flexible coupling crystalline polymer for high-performance aqueous zinc-organic batteries. Chinese Chemical Letters, 2024, 35(9): 109803-. doi: 10.1016/j.cclet.2024.109803
5. [5]
  Yang Li , Xiaoxu Liu , Tianyi Ji , Man Zhang , Xueru Yan , Mengjie Yao , Dawei Sheng , Shaodong Li , Peipei Ren , Zexiang Shen . Potassium ion doped manganese oxide nanoscrolls enhanced the performance of aqueous zinc-ion batteries. Chinese Chemical Letters, 2025, 36(1): 109551-. doi: 10.1016/j.cclet.2024.109551
6. [6]
  Xiaoxi Zhao , Qingyun Dou , Bingjun Yang , Qunji Xue , Xingbin Yan . Intelligent structure modulator for enhancing wide-temperature compatibility of aqueous zinc-ion batteries. Chinese Chemical Letters, 2026, 37(5): 110952-. doi: 10.1016/j.cclet.2025.110952
7. [7]
  Tong Peng , Yupeng Xing , Lan Mu , Chenggang Wang , Ning Zhao , Wenbo Liao , Jianlei Li , Gang Zhao . Recent research on aqueous zinc-ion batteries and progress in optimizing full-cell performance. Chinese Chemical Letters, 2025, 36(6): 110039-. doi: 10.1016/j.cclet.2024.110039
8. [8]
  Yifei Pei , Yong Liu , Chunyang Kong , Zhihui Jia , Kaijia Feng , Yibo Xing , Mingliang He , Xiujie Gao , Ruxia Liu , Xianming Liu , Kunming Pan , Qiaobao Zhang . Graphene-based composites as the cathodes for high-performance aqueous zinc-ion batteries: Applications and perspectives. Chinese Chemical Letters, 2026, 37(4): 110726-. doi: 10.1016/j.cclet.2024.110726
9. [9]
  Zihan Wang , Meizhen Dai , Pengcheng Song , Wenxuan Liu , Junhua You , Fang Hu , Yusheng Wu , Kai Zhu . Triply stabilized NH₄V₄O₁₀ via glycine pillaring enables universal cathode for outstanding rate aqueous zinc-ion batteries and stable aqueous ammonium-ion batteries. Chinese Chemical Letters, 2026, 37(4): 111729-. doi: 10.1016/j.cclet.2025.111729
10. [10]
  Qiao Li , Yijian Chen , Meihua Zhu , Houhou Huang , Fu-Quan Bai , Linglong Hu , Rui Gao , Hongji Xu , Chaoqun Qu , Ming Feng . Constructing robust anode/electrolyte interface by additive in hydrogel to achieve high utilization of Zn anode. Chinese Chemical Letters, 2026, 37(4): 111754-. doi: 10.1016/j.cclet.2025.111754
11. [11]
  Long Huang , Jian Pu , Yunyu Zhao , Xiangxiang Fang , Yingjian Yu , Yuan Li , Jinyan Ma , Yuejin Zhu , Fang Hu , Chuang Yue . Phosphorus-doped carbon as an effective protective layer for advanced aqueous zinc-ion batteries. Chinese Chemical Letters, 2025, 36(8): 110989-. doi: 10.1016/j.cclet.2025.110989
12. [12]
  Renming Liu , Ze Gao , Linglong Hu , Daming Yang , Ming Feng , Dan Luo . Hydrophobic protective layer with ultra-long carbon chain for high-performance aqueous zinc ion batteries. Chinese Chemical Letters, 2026, 37(2): 111491-. doi: 10.1016/j.cclet.2025.111491
13. [13]
  Wenjie Liu , Chuanlin Li , Dingzheng Li , Guangmeng Qu , Mengzhen Kong , Jing Zhang , Xiao Wang , Chenggang Wang , Xijin Xu . Constructing zinc-tin alloy interface for highly stable alkaline zinc anode. Chinese Chemical Letters, 2025, 36(7): 110152-. doi: 10.1016/j.cclet.2024.110152
14. [14]
  Mengdan Tian , Chuanzheng Zhu , Kun Luo . Hybrid organic-inorganic modification on tunnel-structured α-MnO₂ for high-performance aqueous zinc-ion battery. Chinese Chemical Letters, 2026, 37(3): 110702-. doi: 10.1016/j.cclet.2024.110702
15. [15]
  Mengxiao Yang , Haicheng Huang , Shiyi Shen , Xinxin Liu , Mengyu Liu , Jiahua Guo , Fenghui Yang , Baoli Zha , Jiansheng Wu , Sheng Li , Fengwei Huo . Flexible aqueous zinc-ion battery with low-temperature resistant leather gel electrolyte. Chinese Chemical Letters, 2025, 36(6): 109988-. doi: 10.1016/j.cclet.2024.109988
16. [16]
  Xinxiu Yan , Xizhe Huang , Yangyang Liu , Weishang Jia , Hualin Chen , Qi Yao , Tao Chen . Hyperbranched polyamidoamine protective layer with phosphate and carboxyl groups for dendrite-free Zn metal anodes. Chinese Chemical Letters, 2024, 35(10): 109426-. doi: 10.1016/j.cclet.2023.109426
17. [17]
  Zerui Deng , Xincheng Liang , Xingfa Chen , Yuquan Gou , Anning Wang , Peixin Xie , Qian Liu , Huan Wen , Shibin Yin . The role of ammonium formate electrolyte additive for aqueous zinc-ion batteries: Inducing Zn(002) deposition and suppressing hydrogen evolution. Chinese Journal of Structural Chemistry, 2025, 44(11): 100706-100706. doi: 10.1016/j.cjsc.2025.100706
18. [18]
  Peng Wang , Guanyu Zhao , Yicai Pan , Yujing Li , Chenxi Fu , Shipeng Sun , Junqi Gai , Jinping Mu , Xue Bai , Xiaohui Li , Jinfeng Sun , Xiaodong Shi , Rui He . Dual-salt electrolyte strategy enables stable interface reaction and high-performance lithium-ion batteries at low temperature. Chinese Chemical Letters, 2025, 36(11): 111190-. doi: 10.1016/j.cclet.2025.111190
19. [19]
  Li Lin , Song-Lin Tian , Zhen-Yu Hu , Yu Zhang , Li-Min Chang , Jia-Jun Wang , Wan-Qiang Liu , Qing-Shuang Wang , Fang Wang . Molecular crowding electrolytes for stabilizing Zn metal anode in rechargeable aqueous batteries. Chinese Chemical Letters, 2024, 35(7): 109802-. doi: 10.1016/j.cclet.2024.109802
20. [20]
  Liang Wang , Weitao Li , Lei Zheng , Mengmin Jia , Dai-Huo Liu , Dongmei Dai , Zhuangzhuang Zhang , Chunyu Ma , Bao Wang , Shengli Zhang , Li Su , Bao Li . Hemin with strong adsorption on zinc anode as a multi-functional interface layer for highly reversible Zn-ion batteries. Chinese Chemical Letters, 2026, 37(1): 111458-. doi: 10.1016/j.cclet.2025.111458

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(7)
HTML views(0)

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