Citation: Zhongqiu Jia, Fangya Guo, Tianxiang Yang, Shibo Hao, Biying Zhang, Zenan Hu, Leilei Li, Fang Wang, Tingfeng Yi. Dual electrode interphases from high-concentration Zn(OTf)₂ electrolyte: Decoupled voltage retention in Li₃V₂(PO₄)₃ and long-term Zn cycling stability[J]. Chinese Chemical Letters, ;2026, 37(10): 112178. doi: 10.1016/j.cclet.2025.112178 shu

Dual electrode interphases from high-concentration Zn(OTf)₂ electrolyte: Decoupled voltage retention in Li₃V₂(PO₄)₃ and long-term Zn cycling stability

Zhongqiu Jia ^a ,
Fangya Guo ^a ,
Tianxiang Yang ^a ,
Shibo Hao ^a ,
Biying Zhang ^a ,
Zenan Hu ^a ,
Leilei Li ^a ,
Fang Wang ^{a, c, *,} ,
Tingfeng Yi ^{b, *,}

a.
School of School of Energy and Chemical Engineering, Luoyang Institute of Science and Technology, Luoyang 471023, China
b.
Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province, School of Resources and Materials, Northeastern University at Qinhuangdao, Qinhuangdao 066004, China
c.
Henan Province International Joint Laboratory of Materials for Solar Energy Conversion and Lithium Sodium based Battery, Luoyang 471023, China

wangfang1116@163.com

yitingfeng@neuq.edu.cn

Received Date: 6 October 2025
Revised Date: 21 November 2025
Accepted Date: 26 November 2025
Available Online: 26 November 2025

Figures(5)

Aqueous zinc batteries tend to be safe, low-cost, and environmentally friendly. An aqueous cell coupling zinc metal anode and polyanion cathode provides high voltage. However, water-induced side reactions on zinc electrodes, as well as the decomposition of polyanionic cathode, limit the stability of the system. The application of water-in-salt (WiS) electrolytes offers a viable alternative. However, the solubility of conventional zinc salts with weak acidity is low. Herein, we increased the concentration of Zn(OTf)₂ to 10 m (mol/kg_water) by introducing saturated betaine (BT) as a cosolvent. In the 10 m Zn(OTf)₂/13 m BT electrolyte, the high salt concentration and the interactions between betaine and water effectively lower water activity. Moreover, betaine participates in the solvation structure of zinc ions, facilitating the formation of protective interphases on both the zinc anode and the Li₃V₂(PO₄)₃ cathode, thereby suppressing side reactions and cathode decomposition. As a result, the electrolyte enables reversible Zn plating/stripping over 2900 h. The Li₃V₂(PO₄)₃ cathode also maintains two pairs of redox reactions at high voltage of 1.8 V/1.7 V and 1.4 V/1.3 V, demonstrating excellent rate capability and stable cycling performance.
- Aqueous zinc batteries,
- High voltage,
- Li₃V₂(PO₄)₃,
- Betaine,
- High-concentration electrolyte
1. [1]
  M. Li, J. Lu, X. Ji, et al., Nat. Rev. Mater. 5 (2020) 276–294. doi: 10.1038/s41578-019-0166-4
2. [2]
  Y. Liang, Y. Yao, Nat. Rev. Mater. 8 (2022) 109–122. doi: 10.1038/s41578-022-00511-3
3. [3]
  J.X. Jia, C. Liu, Z.G. Neale, et al. Chem. Rev. 120 (2020) 7795–7866. doi: 10.1021/acs.chemrev.9b00628
4. [4]
  H. Li, S. Li, R. Hou, et al., Chem. Soc. Rev. 53 (2024) 7742–7783. doi: 10.1039/d4cs00343h
5. [5]
  D. Chao, S.Z. Qiao, Joule 4 (2020) 1846–1851. doi: 10.1016/j.joule.2020.07.023
6. [6]
  L. Suo, O. Borodin, T. Gao, et al., Science 350 (2015) 938–943. doi: 10.1126/science.aab1595
7. [7]
  M. Kumar, T.C. Nagaiah. Energy Stor. Mater. 44 (2022) 102103.
8. [8]
  T. Liu, K.T. Li, J. Wang, et al., Energy Stor. Mater. 41 (2021) 133–140.
9. [9]
  C. Zhang, J. Holoubek, X. Wu, et al., Chem. Commun. 54 (2018) 14097–14099. doi: 10.1039/c8cc07730d
10. [10]
  W. Fei, O. Borodin, G. Tao, et al., Nat. Mater. 17 (2018) 180–185. doi: 10.1038/nmat5045
11. [11]
  M. Kong, C. Li, X. Zhang, et al., Chin. Chem. Lett. 37 (2026) 111868. doi: 10.1016/j.cclet.2025.111868
12. [12]
  W. Fan, S. Tian, L. Qin, et al., J. Am. Chem. Soc 147 (2025), 18694–18703. doi: 10.1021/jacs.5c01648
13. [13]
  M. Tian, C. Zhu, K. Luo, Chin. Chem. Lett. 37 (2026) 110702. doi: 10.1016/j.cclet.2024.110702
14. [14]
  D. Narsimulu, R. Shanthappa, H. Bandi, et al., ACS Sustain. Chem. Eng. 11 (2023) 12571–12582. doi: 10.1021/acssuschemeng.3c01954
15. [15]
  M. Yan, P. He, Y. Chen, et al., Adv. Mater. 30 (2018) 1703725. doi: 10.1002/adma.201703725
16. [16]
  F. Zhang, T. Liao, H. Peng, et al., J. Am. Chem. Soc. 146 (2024) 10812–10821. doi: 10.1021/jacs.4c01188
17. [17]
  W. Li, K. Wang, S. Cheng, et al., Energy Stor. Mater. 15 (2018) 14–21.
18. [18]
  F. Wang, E. Hu, W. Sun, et al., Energy Environ. Sci. 11 (2018) 3168–3175. doi: 10.1039/c8ee01883a
19. [19]
  F. Wan, Y. Zhang, L. Zhang, et al., Angew. Chem. Int. Ed. 58 (2019) 7062–7067. doi: 10.1002/anie.201902679
20. [20]
  Z. Liu, Q. Yang, D. Wang, et al., Adv. Energy Mater. 9 (2019) 1902473. doi: 10.1002/aenm.201902473
21. [21]
  K. Zhu, Z. Sun, P. Liu, et al., J. Energy Chem. 63 (2021) 239–245. doi: 10.1016/j.jechem.2021.03.051
22. [22]
  D. Kundu, P. Oberholzer, C. Glaros, et al., Chem. Mater. 30 (2018) 3874–3881. doi: 10.1021/acs.chemmater.8b01317
23. [23]
  J. Cui, Z. Guo, J. Yi, et al., ChemSusChem. 13 (2020) 2160–2185. doi: 10.1002/cssc.201903265
24. [24]
  P. Cai, G. Wang, K. Chen, Z. et al., J. Power Sources 428 (2019) 37–43. doi: 10.1016/j.jpowsour.2019.04.103
25. [25]
  W. Wang, V. Balland, M. Branca, B. Limoges, J. Am. Chem. Soc. 146 (2024) 15230–15250. doi: 10.1021/jacs.4c02364
26. [26]
  A. Padhi, K. Nanjundaswamy, J, Goodenough, J. Electrochem. Soc. 144 (1997) 1188–1194. doi: 10.1149/1.1837571
27. [27]
  Z. Jia, X. Yang, H.Y. Shi, et al., Chem. Commun. 58 (2022) 5905–5908. doi: 10.1039/d2cc00946c
28. [28]
  H.Y. Shi, Y. Song, Z. Qin, et al., Angew. Chem. Int. Ed. 58 (2019) 16057–16061. doi: 10.1002/anie.201908853
29. [29]
  C. Li, R. Kingsbury, L. Zhou, et al., ACS Energy Lett. 7 (2022) 533–540. doi: 10.1021/acsenergylett.1c02514
30. [30]
  Z. Jia, F. Wang, F. Guo, et al., ACS Sustain. Chem. Eng. 12 (2024) 8671–8677. doi: 10.1021/acssuschemeng.4c00559
31. [31]
  F. Wang, L.E. Blanc, Q. Li, et al., Adv. Energy Mater. 11 (2021) 2102016. doi: 10.1002/aenm.202102016
32. [32]
  Wan F., Zhang Y., Zhang L.,et al., Angew. Chem. Int. Ed. 58 (2019), 7062–7067. doi: 10.1002/anie.201902679
33. [33]
  Q. Ni, H. Jiang, S. Sandstrom, et al., Adv. Funct. Mater. 30 (2020) 2003511. doi: 10.1002/adfm.202003511
34. [34]
  F. Wang, O. Borodin, T. Gao, et al., Joule 4 (2020) 1557–1574. doi: 10.1364/josaa.395220
35. [35]
  Z. Jia, W. Zhao, S. Hu, et al., Chem. Commun. 58 (2022) 8504–8507. doi: 10.1039/d2cc02553a
36. [36]
  Y. Yang, S. Liang, B. Lu, et al., Energy Environ. Sci. 15 (2022) 1192–1200. doi: 10.1039/d1ee03268b
37. [37]
  C. Li, H. Li, X. Ren, et al., ACS Nano 19 (2025) 2633–2640. doi: 10.1021/acsnano.4c14451
38. [38]
  K. Zhou, Gao. Liu, X. Yu, et al., J. Am. Chem. Soc. 146 (2024) 9455–9464. doi: 10.1021/jacs.4c02150
39. [39]
  T. Qin, K. Li, Y. Liu, et al., Adv. Energy Mater. 13 (2023) 2300733. doi: 10.1002/aenm.202300733
1. [1]
  Xiaojuan Chen , Yanwei Ma , Yiwen Lu , Huimin Zhang , Baozhu Yang , Qi Liu . A high-performance chemically self-charging aqueous zinc battery using a porous organic polymer cathode. Chinese Chemical Letters, 2026, 37(3): 110666-. doi: 10.1016/j.cclet.2024.110666
2. [2]
  Zhen-Zhen Dong , Jin-Hao Zhang , Lin Zhu , Xiao-Zhong Fan , Zhen-Guo Liu , Yi-Bo Yan , Long Kong . Attenuating reductive decomposition of fluorinated electrolytes for high-voltage lithium metal batteries. Chinese Chemical Letters, 2025, 36(4): 109773-. doi: 10.1016/j.cclet.2024.109773
3. [3]
  Xiangkang Jiang , Zhixing Wang , Hong Dong , Xiang Zhang , Jin Hu , Manman Chu , Yanshuai Hong , Lei Xu , Wenjie Peng , Xiqian Yu , Jiexi Wang . An in-depth understanding of Al doping homogeneity affecting the performance of LiCoO₂ at cut-off voltage over 4.6 V. Chinese Chemical Letters, 2024, 35(12): 109553-. doi: 10.1016/j.cclet.2024.109553
4. [4]
  Ruofan Yin , Zhaoxin Guo , Rui Liu , Xian-Sen Tao . Ultrafast synthesis of Na₃V₂(PO₄)₃ cathode for high performance sodium-ion batteries. Chinese Chemical Letters, 2025, 36(2): 109643-. doi: 10.1016/j.cclet.2024.109643
5. [5]
  Lingjiang Kou , Yong Wang , Jiajia Song , Taotao Ai , Wenhu Li , Mohammad Yeganeh Ghotbi , Panya Wattanapaphawong , Koji Kajiyoshi . Mini review: Strategies for enhancing stability of high-voltage cathode materials in aqueous zinc-ion batteries. Chinese Chemical Letters, 2025, 36(1): 110368-. doi: 10.1016/j.cclet.2024.110368
6. [6]
  Zhe Wang , Li-Peng Hou , Qian-Kui Zhang , Nan Yao , Aibing Chen , Jia-Qi Huang , Xue-Qiang Zhang . High-performance localized high-concentration electrolytes by diluent design for long-cycling lithium metal batteries. Chinese Chemical Letters, 2024, 35(4): 108570-. doi: 10.1016/j.cclet.2023.108570
7. [7]
  Shengyu Zhao , Xuan Yu , Yufeng Zhao . A water-stable high-voltage P3-type cathode for sodium-ion batteries. Chinese Chemical Letters, 2024, 35(9): 109933-. doi: 10.1016/j.cclet.2024.109933
8. [8]
  Yue Wang , Caixia Xu , Xingtao Tian , Siyu Wang , Yan Zhao . Challenges and Modification Strategies of High-Voltage Cathode Materials for Li-ion Batteries. Chinese Journal of Structural Chemistry, 2023, 42(10): 100167-100167. doi: 10.1016/j.cjsc.2023.100167
9. [9]
  Mengzhen Kong , Chuanlin Li , Xixi Zhang , Na Li , Jing Zhang , Wenjie Liu , Dingzheng Li , Chenggang Wang , Xijin Xu . High-voltage mild aqueous zinc-manganese battery with two-electron transfer accessed by aluminum ion regulation. Chinese Chemical Letters, 2026, 37(8): 111868-. doi: 10.1016/j.cclet.2025.111868
10. [10]
  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
11. [11]
  Tong Su , Yue Wang , Qizhen Zhu , Mengyao Xu , Ning Qiao , Bin Xu . Multiple conductive network for KTi₂(PO₄)₃ anode based on MXene as a binder for high-performance potassium storage. Chinese Chemical Letters, 2024, 35(8): 109191-. doi: 10.1016/j.cclet.2023.109191
12. [12]
  Jiayu Bai , Songjie Hu , Lirong Feng , Xinhui Jin , Dong Wang , Kai Zhang , Xiaohui Guo . Manganese vanadium oxide composite as a cathode for high-performance aqueous zinc-ion batteries. Chinese Chemical Letters, 2024, 35(9): 109326-. doi: 10.1016/j.cclet.2023.109326
13. [13]
  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
14. [14]
  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
15. [15]
  Jiaxuan Liu , Nan Zhang , Huiming Shi , Zhipeng He , Zhiyu Zhang , Dianlong Wang , Huakun Liu , Shixue Dou , Bo Wang . Single crystal P2-type layered cathodes with optimized crystal plane orientation improved high voltage stability for sodium-ion batteries. Chinese Chemical Letters, 2026, 37(5): 110892-. doi: 10.1016/j.cclet.2025.110892
16. [16]
  Mei-Chen Liu , Qing-Song Liu , Yi-Zhou Quan , Jia-Ling Yu , Gang Wu , Xiu-Li Wang , Yu-Zhong Wang . Phosphorus-silicon-integrated electrolyte additive boosts cycling performance and safety of high-voltage lithium-ion batteries. Chinese Chemical Letters, 2024, 35(8): 109123-. doi: 10.1016/j.cclet.2023.109123
17. [17]
  Tao Long , Peng Chen , Bin Feng , Caili Yang , Kairong Wang , Yulei Wang , Can Chen , Yaping Wang , Ruotong Li , Meng Wu , Minhuan Lan , Wei Kong Pang , Jian-Fang Wu , Yuan-Li Ding . Reinforced concrete-like Na_3.5V_1.5Mn_0.5(PO₄)₃@graphene hybrids with hierarchical porosity as durable and high-rate sodium-ion battery cathode. Chinese Chemical Letters, 2024, 35(4): 109267-. doi: 10.1016/j.cclet.2023.109267
18. [18]
  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
19. [19]
  Chengjun Wu , Yajiang Wang , Xiaoduo Jiang , Huixiong Jiang , Jin-Hang Liu , Ping Yan , Hai-Yan Hu , Yao Xiao , Xiudong Chen . Dual-guest co–intercalation engineering enables high-energy and long-life aqueous zinc-ion batteries. Chinese Chemical Letters, 2026, 37(10): 112787-. doi: 10.1016/j.cclet.2026.112787
20. [20]
  Le Li , Shaofeng Jia , Shi Yue , Yuanyuan Yang , Chao Tan , Conghui Wang , Hengwei Qiu , Yongqiang Ji , Minghui Cao , Zige Tai , Dan Zhang . Vanadium doping inhibit the Jahn−Teller effect of Mn³⁺ for high-performance aqueous zinc ion battery. Chinese Chemical Letters, 2025, 36(10): 111009-. doi: 10.1016/j.cclet.2025.111009

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(3)
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

Dual electrode interphases from high-concentration Zn(OTf)2 electrolyte: Decoupled voltage retention in Li3V2(PO4)3 and long-term Zn cycling stability

Metrics

通讯作者: 陈斌, bchen63@163.com

Dual electrode interphases from high-concentration Zn(OTf)₂ electrolyte: Decoupled voltage retention in Li₃V₂(PO₄)₃ and long-term Zn cycling stability