Citation: Jiao Wang, Shuang-Yan Lang, Zhen-Zhen Shen, Gui-Xian Liu, Jian-Xin Tian, Yuan Li, Rui-Zhi Liu, Rui Wen. In situ imaging of the interfacial processes manipulated by salt concentration on zinc anodes in zinc metal batteries[J]. Chinese Chemical Letters, ;2025, 36(4): 109815. doi: 10.1016/j.cclet.2024.109815 shu

In situ imaging of the interfacial processes manipulated by salt concentration on zinc anodes in zinc metal batteries

Jiao Wang ^{a, b} ,
Shuang-Yan Lang ^{a, b} ,
Zhen-Zhen Shen ^{a, b} ,
Gui-Xian Liu ^{a, b} ,
Jian-Xin Tian ^{a, b} ,
Yuan Li ^{a, b} ,
Rui-Zhi Liu ^{a, b} ,
Rui Wen ^{a, b, *,}

a.
CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Beijing National Laboratory for Molecular Sciences, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
b.
University of Chinese Academy of Sciences, Beijing 100049, China

ruiwen@iccas.ac.cn

Received Date: 2 March 2024
Accepted Date: 22 March 2024
Available Online: 23 March 2024

Figures(5)

Unstable electrode/electrolyte interfaces and heterogeneous Zn deposition would reduce the Coulombic efficiency and cycle life of Zn metal batteries (ZMBs). Applying water-in-salt (WIS) electrolytes has proven to be an effective strategy to address the above issues. However, an understanding of the reaction mechanisms on the Zn anode at nanoscale is still elusive. Here we utilize in situ atomic force microscopy to visualize the solid electrolyte interphase (SEI) formation and Zn deposition/dissolution processes in WIS electrolyte and construct relationships between interfacial behavior and electrochemical performance. The formation processes, chemical properties, and structure of the on-site formed SEI are deeply explored. The SEI with a “plum-pudding” model can guide uniform Zn deposition and reversible dissolution. Mechanistic understanding of the interfacial evolution of the SEI layer and Zn deposition/dissolution has been achieved and will benefit the structural optimization and interfacial engineering of ZMBs.
- In situ AFM,
- Interfacial processes,
- Solid electrolyte interphase,
- Water-in-salt,
- Zn metal batteries
1. [1]
  C.S. Lai, Y. Jia, L.L. Lai, et al., Renew. Sustain. Energy Rev. 78 (2017) 439–451. doi: 10.1016/j.rser.2017.04.078
2. [2]
  J. Zheng, M.S. Kim, Z. Tu, et al., Chem. Soc. Rev. 49 (2020) 2701–2750. doi: 10.1039/c9cs00883g
3. [3]
  H. Kim, J. Hong, K.Y. Park, et al., Chem. Soc. Rev. 49 (2020) 2701–2750.
4. [4]
  A. Yoshino, Angew. Chem. Int. Ed. 51 (2012) 5798–5800. doi: 10.1002/anie.201105006
5. [5]
  L. Chen, C. Chen, L. Jin, et al., Energy Environ. Sci. 14 (2021) 955–964. doi: 10.1039/d0ee02777d
6. [6]
  Z. Tie, Y. Zhang, J. Zhu, S. Bi, Z. Niu, J. Am. Chem. Soc. 144 (2022) 10301–10308. doi: 10.1021/jacs.2c01485
7. [7]
  J. Zheng, D.C. Bock, T. Tang, et al., Nat. Energy 6 (2021) 398–406. doi: 10.1038/s41560-021-00797-7
8. [8]
  C. Li, R. Kingsbury, A.S. Thind, A. Shyamsunder, et al., Nat. Commun. 14 (2023) 3067.
9. [9]
  Y. Wang, J. Yin, J. Zhu, Chin. J. Chem. 40 (2022) 973–988. doi: 10.1002/cjoc.202100791
10. [10]
  M. Zhang, H. Peng, K. Sun, et al., Chin. J. Chem. 40 (2022) 2763–2772. doi: 10.1002/cjoc.202200217
11. [11]
  X. Zheng, Z. Liu, J. Sun, et al., Nat. Commun. 14 (2023) 76. doi: 10.1038/s41467-022-35630-6
12. [12]
  Q. Yang, Q. Li, Z. Liu, et al., Adv. Mater. 32 (2020) 2001854.
13. [13]
  T. Huang, K. Xu, N. Jia, et al., Adv. Mater. 35 (2023) 2205206.
14. [14]
  S. Cai, G. Chang, J. Hu, et al., Chin. J. Chem. 41 (2023) 1697–1704. doi: 10.1002/cjoc.202200799
15. [15]
  Z. Yi, G. Chen, F. Hou, L. Wang, J. Liang, Adv. Energy Mater. 11 (2021) 2003065. doi: 10.1002/aenm.202003065
16. [16]
  L. Kang, M. Cui, F. Jiang, et al., Adv. Energy Mater. 8 (2018) 1801090.
17. [17]
  X. Wu, Y. Dai, N.W. Li, X.C. Chen, L. Yu, eScience (2023) 100173.
18. [18]
  W. Zhang, G. He, Angew. Chem. Int. Ed. 62 (2023) e202218466.
19. [19]
  X. Zeng, J. Mao, J. Hao, et al., Adv. Mater. 33 (2021) 2007416.
20. [20]
  P. Xiong, Y. Kang, N. Yao, et al., ACS Energy Lett. 8 (2023) 1613–1625. doi: 10.1021/acsenergylett.3c00154
21. [21]
  S. Jin, F. Duan, X. Wu, et al., Small 18 (2022) 2205462.
22. [22]
  L. Suo, O. Borodin, W. Sun, et al., Angew. Chem. Int. Ed. 55 (2016) 7136–7141. doi: 10.1002/anie.201602397
23. [23]
  J. Wang, J.X. Tian, G.X. Liu, Z.Z. Shen, R. Wen, Small Methods 7 (2023) 2300392. doi: 10.1002/smtd.202300392
24. [24]
  E. Hu, X.Q. Yang, Nat. Mater. 17 (2018) 480–481. doi: 10.1038/s41563-018-0090-9
25. [25]
  K. Gao, S. Li, J. Liu, et al., Adv. Funct. Mater. 33 (2023) 2307641. doi: 10.1002/adfm.202307641
26. [26]
  L. Cao, D. Li, T. Pollard, et al., Nat. Nanotechnol. 16 (2021) 902–910. doi: 10.1038/s41565-021-00905-4
27. [27]
  W. Wang, S. Chen, X. Liao, et al., Nat. Commun. 14 (2023) 5443. doi: 10.3390/rs15235443
28. [28]
  S. Di, X. Nie, G. Ma, et al., Energy Stor. Mater. 43 (2021) 375–382.
29. [29]
  D. Li, L. Cao, T. Deng, S. Liu, C. Wang, Angew. Chem. Int. Ed. 60 (2021) 13035–13041. doi: 10.1002/anie.202103390
30. [30]
  H. Wu, H. Jia, C. Wang, J.G. Zhang, W. Xu, Adv. Energy Mater. 11 (2021) 2003092. doi: 10.1002/aenm.202003092
31. [31]
  H. Qiu, X. Du, J. Zhao, et al., Nat. Commun. 10 (2019) 5374. doi: 10.1038/s41467-019-13436-3
32. [32]
  Y. Chu, S. Zhang, S. Wu, et al., Energy Environ. Sci. 14 (2021) 3609–3620. doi: 10.1039/d1ee00308a
33. [33]
  Y. An, Y. Tian, K. Zhang, et al., Adv. Funct. Mater. 31 (2021) 2101886. doi: 10.1002/adfm.202101886
34. [34]
  W. Hu, J. Ju, N. Deng, et al., J. Mater. Chem. A 9 (2021) 25750–25772. doi: 10.1039/d1ta08184e
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