Citation: Fan Zhang, Zizhu Guo, Jin Wang, Dan Sun, Xiaobing Huang, Qi Zhang, Yougen Tang, Yusi Yang, Haiyan Wang. Durable anode-free lithium metal batteries enabled by a lithiophilic Cu-Zn Solid-Solution with accelerated interfacial Li⁺ diffusion kinetics[J]. Chinese Chemical Letters, ;2026, 37(10): 112057. doi: 10.1016/j.cclet.2025.112057 shu

Durable anode-free lithium metal batteries enabled by a lithiophilic Cu-Zn Solid-Solution with accelerated interfacial Li⁺ diffusion kinetics

Fan Zhang ^{a, 1} ,
Zizhu Guo ^{a, 1} ,
Jin Wang ^a ,
Dan Sun ^a ,
Xiaobing Huang ^{b, *,} ,
Qi Zhang ^a ,
Yougen Tang ^a ,
Yusi Yang ^{a, *,} ,
Haiyan Wang ^{a, *,}

a.
Hunan Provincial Key Laboratory of Chemical Power Sources, College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
b.
College of Chemistry and Chemical Engineering, Hunan University of Arts and Science, Changde 415000, China

hxb220170@126.com

nameyys@163.com

wanghy419@csu.edu.cn

Received Date: 24 September 2025
Revised Date: 29 October 2025
Accepted Date: 3 November 2025
Available Online: 6 November 2025

Figures(6)

Cu-Zn solid solutions are investigated as advanced current collector materials for anode-free Li metal batteries (AFLMBs), addressing the limited lithiophilicity and slow Li⁺ diffusion kinetics inherent to conventional Cu foil. Benefiting from the uniform distribution of lithiophilic Zn, Cu-Zn solid solutions demonstrated enhanced lithiophilicity and accelerated Li⁺ diffusion, which effectively facilitated uniform and reversible lithium deposition. First-principles calculations confirmed that Cu-Zn solid solutions, particularly Cu₆₂Zn₃₈, exhibited stronger Li adsorption and reduced diffusion barriers compared to Cu. Unlike alloy-prone metal coatings (e.g., Cu@Zn and thermally processed Cu@Zn) that sacrifice interfacial stability for lithiophilicity, Cu-Zn solid solution maintains robust electrode-electrolyte interfaces due to its alloying inertness. Ex-situ SEM and COMSOL simulations revealed dendrite-suppressed and homogeneous Li deposition on Cu₆₂Zn₃₈. In anode-free full cells, Cu₆₂Zn₃₈ achieves a capacity retention of 55.1% after 150 cycles, far exceeding Cu foil (13.8%). This work establishes Cu-Zn solid solutions current collectors as a scalable solution for high-energy-density AFLMBs.
- Anode-free lithium metal batteries,
- Solid solution,
- Interfacial stability,
- Lithiophilicity,
- High energy density batteries
1. [1]
  S. Yang, Y. Wang, H. Pan, P. He, H. Zhou, Nature 636 (2024) 309–321. doi: 10.1038/s41586-024-08117-1
2. [2]
  G. Harper, R. Sommerville, E. Kendrick, et al., Nature 575 (2019) 75–86. doi: 10.1038/s41586-019-1682-5
3. [3]
  J. Xiao, F. Shi, T. Glossmann, C. Burnett, Z. Liu, Nat. Energy 8 (2023) 329–339. doi: 10.1038/s41560-023-01221-y
4. [4]
  F. Schomburg, B. Heidrich, S. Wennemar, et al., Energ. Environ. Sci. 17 (2024) 2686–2733. doi: 10.1039/d3ee03559j
5. [5]
  J. Zhang, W. Xu, J. Xiao, X. Cao, J. Liu, Chem. Rev. 120 (2020) 13312–13348. doi: 10.1021/acs.chemrev.0c00275
6. [6]
  H. Wan, J. Xu, C. Wang, Nat. Rev. Chem. 8 (2024) 30–44.
7. [7]
  S. Huo, L. Wang, B. Su, et al., Adv. Mater. 36 (2024) 2411757. doi: 10.1002/adma.202411757
8. [8]
  Y. An, Y. Zeng, D. Luan, X.W.D. Lou, Matter. 7 (2024) 1466–1502. doi: 10.1016/j.matt.2024.02.012
9. [9]
  L. Dong, S. Zhong, B. Yuan, et al., Angew. Chem. Int. Ed. 135 (2023) e202301073. doi: 10.1002/anie.202301073
10. [10]
  S. Nanda, A. Gupta, A. Manthiram, Adv. Energy Mater. 11 (2021) 2000804. doi: 10.1002/aenm.202000804
11. [11]
  Y. Zhou, P. Wang, K. Wang, et al., Adv. Funct. Mater. 35 (2025) 2424022. doi: 10.1002/adfm.202424022
12. [12]
  J. Shi, C. Xu, J. Lai, et al., Angew. Chem. Int. Ed. 135 (2023) e202218151. doi: 10.1002/anie.202218151
13. [13]
  M. Mao, X. Ji, Q. Wang, et al., Nat. Commun. 14 (2023) 1082. doi: 10.1038/s41467-023-36853-x
14. [14]
  H. Su, H. Zhang, Z. Chen, et al., Chin. Chem. Lett. 34 (2023) 108640. doi: 10.1016/j.cclet.2023.108640
15. [15]
  K. Peng, X. Wang, X. Yan, Chin. Chem. Lett. 35 (2024) 109274. doi: 10.1016/j.cclet.2023.109274
16. [16]
  J. Sun, S. Zhang, J. Li, B. Xie, J. Ma, S. Dong, G. Cui, Adv. Mater. 35 (2023) 2209404. doi: 10.1002/adma.202209404
17. [17]
  Q. Zhao, S. Stalin, L.A. Archer, Joule 5 (2021) 1119–1142. doi: 10.1016/j.joule.2021.03.024
18. [18]
  S. Zhang, H. Liao, Z. Liu, C. Yan, J. Huang, Chin. Chem. Lett. 35 (2024) 109284. doi: 10.1016/j.cclet.2023.109284
19. [19]
  X.L. Zhang, L. Ma, Y.P. Cai, J. Fransaer, Q. Zheng, Matter 7 (2024) 583–602.
20. [20]
  Z. Ouyang, S. Wang, Y. Wang, et al., Adv. Mater. 36 (2024) 2407648. doi: 10.1002/adma.202407648
21. [21]
  C.Y. Im, G.Y. Lee, J.G. Kim, J.H. Choi, S.J. Kim, Adv. Mater. 37 (2025) 2501261. doi: 10.1002/adma.202501261
22. [22]
  Z. Ouyang, Y. Wang, S. Wang, et al., Adv. Mater. 36 (2024) 2401114. doi: 10.1002/adma.202401114
23. [23]
  J. Wang, Y. Wang, X. Lu, et al., Adv. Mater. 36 (2024) 2308257. doi: 10.1002/adma.202308257
24. [24]
  H. Kwon, J.H. Lee, Y. Roh, et al., Nat. Commun. 12 (2021) 5537. doi: 10.1038/s41467-021-25848-1
25. [25]
  Y. Wang, Y. Li, X. Wang, et al., Adv. Mater. 37 (2025) 2420373. doi: 10.1002/adma.202420373
26. [26]
  S. Huang, S. Lu, Y. Lv, et al., Nano Res. 16 (2023) 11473–11485. doi: 10.1007/s12274-023-5795-7
27. [27]
  S.K. Merso, T.M. Tekaligne, M.A. Weret, et al., Chem. Eng. J. 486 (2024) 149547.
28. [28]
  T.A. Nigatu, H.K. Bezabh, S.K. Jiang, et al., Electrochim. Acta 443 (2023) 141883. doi: 10.1016/j.electacta.2023.141883
1. [1]
  Zhaojun Chen , Yongqi Wang , Yongshun Liang , Liang Shan , Ying Wang , Jiyue Hou , Ziyi Zhu , Xue Li , Yiyong Zhang . In-situ polymerization technology for all-solid state lithium batteries: Current status and future development. Chinese Chemical Letters, 2026, 37(6): 112020-. doi: 10.1016/j.cclet.2025.112020
2. [2]
  Jianing He , Xiao Wang , Zijian Wang , Ruize Jiang , Ke Wang , Rui Zhang , Huilin Wang , Baokang Geng , Hongyi Gao , Shuyan Song , Hongjie Zhang . Investigation on Cu promotion effect on Ce-based solid solution-anchored Rh single atoms for three-way catalysis. Chinese Chemical Letters, 2025, 36(2): 109640-. doi: 10.1016/j.cclet.2024.109640
3. [3]
  Yaoce Wang , Keyu Zhang , Xinyu Jiang , Binbin Li , Bo Jin , Juan Yang , Xiangyang Zhou , Bin Yang , Yaochun Yao . Micron silicon anodes for superior lithium storage: A view from chemical-mechanical degradation mechanisms to interface electrolyte systematic design. Chinese Chemical Letters, 2026, 37(9): 112631-. doi: 10.1016/j.cclet.2026.112631
4. [4]
  Haiying Lu , Weijie Li . The electrolyte solvation and interfacial chemistry for anode-free sodium metal batteries. Chinese Journal of Structural Chemistry, 2024, 43(11): 100334-100334. doi: 10.1016/j.cjsc.2024.100334
5. [5]
  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
6. [6]
  Jing Guo . Stacking solid-state electrolyte and aluminum pellets for anode-free solid-state batteries. Chinese Chemical Letters, 2025, 36(5): 110764-. doi: 10.1016/j.cclet.2024.110764
7. [7]
  Jiaojiao Deng , Haocheng Li , Fei Zheng , Qingsong Weng , Yu Bai , Xiaoliang Yu , Qianlin Zhang , Qinghua Liang , Baohua Li . A “breathable” 3D lithium host with MnO₂ nanoflake array for long-lifespan anode-free lithium metal batteries. Chinese Chemical Letters, 2026, 37(3): 110681-. doi: 10.1016/j.cclet.2024.110681
8. [8]
  Jialiang Zhu , Yuan Zhong , Bingqing Xu , Gen Zhang . Multiscale interfacial engineering of halide electrolytes for high-performance all-solid-state lithium batteries. Chinese Journal of Structural Chemistry, 2026, 45(4): 100850-100850. doi: 10.1016/j.cjsc.2025.100850
9. [9]
  Bosen Zhang , Yecheng Yan , Zhiyuan Chen , Shuo Yang , Zhi Yang . Ga₂O₃-doped argyrodite sulfide solid electrolyte enhances interface stability of all-solid-state lithium metal batteries. Chinese Chemical Letters, 2026, 37(10): 111952-. doi: 10.1016/j.cclet.2025.111952
10. [10]
  Tianyi Hou , Yunhui Huang , Henghui Xu . Interfacial engineering for advanced solid-state Li-metal batteries. Chinese Journal of Structural Chemistry, 2024, 43(7): 100313-100313. doi: 10.1016/j.cjsc.2024.100313
11. [11]
  Xin Li , Ling Zhang , Yunyan Fan , Shaojing Lin , Yong Lin , Yongsheng Ying , Meijiao Hu , Haiying Gao , Xianri Xu , Zhongbiao Xia , Xinchuan Lin , Junjie Lu , Xiang Han . Carbon interconnected microsized Si film toward high energy room temperature solid-state lithium-ion batteries. Chinese Chemical Letters, 2025, 36(2): 109776-. doi: 10.1016/j.cclet.2024.109776
12. [12]
  Mengwen Wang , Qintao Sun , Yue Liu , Zhengan Yan , Qiyu Xu , Yuchen Wu , Tao Cheng . Impact of lithium nitrate additives on the solid electrolyte interphase in lithium metal batteries. Chinese Journal of Structural Chemistry, 2024, 43(2): 100203-100203. doi: 10.1016/j.cjsc.2023.100203
13. [13]
  Jie Chen , Hannan Chen , Bingbing Tian . Enhancing moisture and electrochemical stability of the Li_5.7PS_4.7Cl_1.3 electrolyte by boron nitride coating for all-solid-state lithium metal batteries. Chinese Chemical Letters, 2025, 36(7): 109775-. doi: 10.1016/j.cclet.2024.109775
14. [14]
  Qingkun Zhu , Yaodong Jin , Bao Zhang , Wei Liu , Haozhe Qin , Lei Ming , Xing Ou . Engineering a triplex ionic transport architecture for high ionic conductivity in solid-state lithium metal batteries. Chinese Chemical Letters, 2026, 37(8): 111411-. doi: 10.1016/j.cclet.2025.111411
15. [15]
  Shuo Zhang , Haitao Liao , Zhi-Qun Liu , Chong Yan , Jia-Qi Huang . Re-evaluating the nano-sized inorganic protective layer on Cu current collector for anode free lithium metal batteries. Chinese Chemical Letters, 2024, 35(7): 109284-. doi: 10.1016/j.cclet.2023.109284
16. [16]
  Ying Li , Ze-Chen Lv , Peng-Fei Wang , Jie Shu , Ping He , Ting-Feng Yi . Constructing stable cathode by g-C₃N₄ nanosheets for high-energy all-solid-state lithium-sulfur batteries. Chinese Chemical Letters, 2026, 37(7): 111110-. doi: 10.1016/j.cclet.2025.111110
17. [17]
  Run Chai , Qiujie Wu , Yongchao Liu , Xiaohui Song , Xuyong Feng , Yi Sun , Hongfa Xiang . A 3D dual layer host with enhanced sodiophilicity as stable anode for high-energy sodium metal batteries. Chinese Chemical Letters, 2025, 36(6): 110007-. doi: 10.1016/j.cclet.2024.110007
18. [18]
  Haotian Zhang , Shengfa Feng , Mufan Cao , Xiong Xiong Liu , Pengcheng Yuan , Yaping Wang , Min Gao , Long Pan , Zhengming Sun . Al₂O₃ coated polyimide porous films enable thin yet strong polymer-in-salt solid-state electrolytes for dendrite-free lithium metal batteries. Chinese Chemical Letters, 2025, 36(8): 111096-. doi: 10.1016/j.cclet.2025.111096
19. [19]
  Xin Xia , Zhong-Qi Zhang , Qing Wen , Pei-Yao Li , Ding-Hao Le , Zhen-Yu Wang , Pan-Pan Dong , Guo-Dong Ren , Jun-Chao Zheng . Metal-organic-framework-based solid-state electrolytes for high-performance lithium metal batteries: Recent advances and prospects. Chinese Chemical Letters, 2026, 37(10): 111653-. doi: 10.1016/j.cclet.2025.111653
20. [20]
  Xinpin Pan , Yongjian Cui , Zhe Wang , Bowen Li , Hailong Wang , Jian Hao , Feng Li , Jing Li . Robust chemo-mechanical stability of additives-free SiO₂ anode realized by honeycomb nanolattice for high performance Li-ion batteries. Chinese Chemical Letters, 2024, 35(10): 109567-. doi: 10.1016/j.cclet.2024.109567

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

Durable anode-free lithium metal batteries enabled by a lithiophilic Cu-Zn Solid-Solution with accelerated interfacial Li+ diffusion kinetics

Metrics

通讯作者: 陈斌, bchen63@163.com

Durable anode-free lithium metal batteries enabled by a lithiophilic Cu-Zn Solid-Solution with accelerated interfacial Li⁺ diffusion kinetics