Citation: Yucheng Wang, Xiaodan Li, Xunhui Xiong, Yuancheng Chen, Yun Cheng, Jianhao Lin, Chuang Ji, Yingyi Yuan. Ferromagnetic filler-induced stable electrode/electrolyte interfaces for solid-state Li metal batteries[J]. Chinese Chemical Letters, ;2026, 37(9): 111528. doi: 10.1016/j.cclet.2025.111528 shu

Ferromagnetic filler-induced stable electrode/electrolyte interfaces for solid-state Li metal batteries

Yucheng Wang ^a ,
Xiaodan Li ^a ,
Xunhui Xiong ^{a, *,} ,
Yuancheng Chen ^a ,
Yun Cheng ^{b, *,} ,
Jianhao Lin ^a ,
Chuang Ji ^a ,
Yingyi Yuan ^a

a.
School of Environment and Energy, Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, South China University of Technology, Guangzhou 510006, China
b.
Guangdong Saffien New Materials Co., Ltd., Qingyuan 511520, China

esxxiong@scut.edu.cn

chengerr@126.com

Received Date: 12 April 2025
Revised Date: 25 June 2025
Accepted Date: 1 July 2025
Available Online: 2 July 2025

Figures(5)

Solid polymer electrolyte (SPEs) modified by inorganic fillers has become a simple and effective strategy to improve ionic conductivity and mechanical strength. However, the uneven charge distribution at the interface of polymer electrolyte/electrode results in unstable interfaces and poor cycle performances. Herein, ferromagnetic (La_0.60Sr_0.40)_0.95Co_0.20Fe_0.80O_3-δ (LSCF) has been firstly proposed as filler for PVDF-based electrolyte (PLSCF) to address these critical challenges in solid-state Li metal battery. It has been demonstrated that LSCF filler cannot only increase the ratio of amorphous phase in the polymer, but also induce the rearrangement of PVDF molecular chains under an applied external magnetic field during the preparation process, which can facilitate the generation of the β-phase and promote the dissociation of Li⁺. The synthesized PLSCF electrolyte exhibits appealing physicochemical properties, including enhanced ionic conductivity (2.09×10⁻⁴ S/cm), reduced activation energy (0.142 eV), and improved mechanical robustness (1.286 MPa), which can contribute to a homogeneous lithium deposition on Li metal anode. Furthermore, LSCF can establish an even electric field at the PLSCF/cathode interface, which helps to weaken the space charging layer and construct a robust cathode/electrolyte interface (CEI). As a result, both solid-state Li/Li symmetric cells and LiNi_0.6Co_0.2Mn_0.2O₂/Li full cells incorporating the PLSCF electrolyte exhibit significantly improved cycling stability and rate capability. This work enriches inorganic fillers to stabilize electrode/electrolyte interface for high-performance solid-state Li metal batteries.
- Solid-state Li metal batteries,
- PVDF polymer electrolyte,
- Ferromagnetic packing,
- Space charge layer,
- Interfacial electric field
1. [1]
  C. Chen, Q. Liang, G. Wang, et al., Adv. Funct. Mater. 32 (2022) 2107249. doi: 10.1002/adfm.202107249
2. [2]
  C. Ji, Q. Zhou, Y. Yuan, et al., Energy Environ. Sci. 17 (2024) 4273–4282. doi: 10.1039/d4ee00970c
3. [3]
  H. Chen, M. Zheng, S. Qian, et al., Carbon Energy 3 (2021) 929–956. doi: 10.1002/cey2.146
4. [4]
  Y. Wang, J. Wang, J. Nai, et al., Chin. Chem. Lett. 35 (2024) 108510. doi: 10.1016/j.cclet.2023.108510
5. [5]
  K. Yang, L. Li, Y. Xiao, et al., Chin. Chem. Lett. 35 (2024) 108451. doi: 10.1016/j.cclet.2023.108451
6. [6]
  X. Li, Q. Liu, Y. Wang, et al., Small 21 (2025) 2411104. doi: 10.1002/smll.202411104
7. [7]
  X. Zhang, S. Wang, C. Xue, et al., Adv. Mater. 31 (2019) 1806082. doi: 10.1002/adma.201806082
8. [8]
  Y. Zhao, Y. Zhang, D. Gosselink, et al., Membranes 2 (2012) 553–564. doi: 10.3390/membranes2030553
9. [9]
  M. Hong, Q. Dong, H. Xie, et al., ACS Energy Lett. 6 (2021) 3753–3760. doi: 10.1021/acsenergylett.1c01554
10. [10]
  M. Zhang, M.B. Gomes, A. Yusuf, et al., Eur. Polym. J. 215 (2024) 113246. doi: 10.1016/j.eurpolymj.2024.113246
11. [11]
  Q. Song, Y. Zhang, J. Liang, et al., Chin. Chem. Lett. 35 (2024) 108797. doi: 10.1016/j.cclet.2023.108797
12. [12]
  R. Yin, Z. Zhang, C. Shi, et al., ACS Appl. Mater. Interfaces 16 (2024) 60142–60150. doi: 10.1021/acsami.4c10917
13. [13]
  D. Kumar, S. Mukherjee, A. Das, J. Appl. Polym. Sci. 141 (2024) e55552. doi: 10.1002/app.55552
14. [14]
  Z. Zhang, Y. Ren, J. Liang, et al., Energy Storage Mater. 71 (2024) 103667. doi: 10.1016/j.ensm.2024.103667
15. [15]
  G. Lu, Y. Zhang, J. Zhang, et al., Carbon Energy 5 (2023) e287. doi: 10.1002/cey2.287
16. [16]
  S. Khurana, S. Negi, A. Chandra, Polym. Test. 96 (2021) 107118. doi: 10.1016/j.polymertesting.2021.107118
17. [17]
  G. Xi, M. Xiao, S. Wang, et al., Adv. Funct. Mater. 31 (2021) 2007598. doi: 10.1002/adfm.202007598
18. [18]
  Y. Wu, Y. Li, Y. Wang, et al., J. Energy Chem. 64 (2022) 62–84. doi: 10.1016/j.jechem.2021.04.007
19. [19]
  X. Li, Y. Wang, Q. Zhou, et al., J. Mater. Chem. A 12 (2024) 7645–7653. doi: 10.1039/d3ta08117f
20. [20]
  S. Zhou, S. Zhong, Y. Dong, et al., Adv. Funct. Mater. 33 (2023) 2214432. doi: 10.1002/adfm.202214432
21. [21]
  Z. Wang, S. Xie, X. Gao, et al., Chin. Chem. Lett. 34 (2023) 108151. doi: 10.1016/j.cclet.2023.108151
22. [22]
  X. An, Y. Liu, K. Yang, et al., Adv. Mater. 36 (2024) 2311195. doi: 10.1002/adma.202311195
23. [23]
  S. Liu, W. Liu, D. Ba, et al., Adv. Mater. 35 (2023) 2110423. doi: 10.1002/adma.202110423
24. [24]
  Q. Zhou, J. Ma, S. Dong, et al., Adv. Mater. 31 (2019) 1902029. doi: 10.1002/adma.201902029
25. [25]
  L. Li, Y. Shan, X. Yang, Mater. Today Commun. 26 (2021) 101910. doi: 10.1016/j.mtcomm.2020.101910
26. [26]
  X. Zhang, T. Liu, S. Zhang, et al., J. Am. Chem. Soc. 139 (2017) 13779–13785. doi: 10.1021/jacs.7b06364
27. [27]
  K. Li, J. Wang, Q. Shen, et al., Adv. Energy Mater. 14 (2024) 2400956. doi: 10.1002/aenm.202400956
28. [28]
  S. Li, S.Q. Zhang, L. Shen, et al., Adv. Sci. 7 (2020) 1903088. doi: 10.1002/advs.201903088
29. [29]
  P. Shi, J. Ma, M. Liu, et al., Nat. Nanotechnol. 18 (2023) 602–610. doi: 10.1038/s41565-023-01341-2
30. [30]
  X. Liu, B. Wen, G. Zhong, et al., Sci. China Mater. 67 (2024) 1947–1955. doi: 10.1007/s40843-024-2915-3
31. [31]
  T.U. Patro, M.V. Mhalgi, D.V. Khakhar, et al., Polymer 49 (2008) 3486–3499. doi: 10.1016/j.polymer.2008.05.034
32. [32]
  Y. Zhu, F. Wang, L. Liu, et al., Energy Environ. Sci. 6 (2013) 618–624. doi: 10.1039/C2EE23564A
33. [33]
  Y. Jin, X. Zong, X. Zhang, et al., J. Power Sources 501 (2021) 230027. doi: 10.1016/j.jpowsour.2021.230027
34. [34]
  Y. Shan, L. Li, X. Yang, ACS Appl. Energ. Mater. 4 (2021) 5101–5112. doi: 10.1021/acsaem.1c00658
35. [35]
  J. Lu, Y. Li, W. Huang, Mater. Res. Bull. 153 (2022) 111880. doi: 10.1016/j.materresbull.2022.111880
36. [36]
  J.P. Serra, R.S. Pinto, J.C. Barbosa, et al., Sustain. Mater. Technol. 25 (2020) e00176.
37. [37]
  R. Mishra, S.K. Singh, H. Gupta, et al., Energy Fuels 35 (2021) 15153–15165. doi: 10.1021/acs.energyfuels.1c02114
38. [38]
  P. Martins, A.C. Lopes, S. Lanceros-Mendez, Prog. Polym. Sci. 39 (2014) 683–706. doi: 10.1016/j.progpolymsci.2013.07.006
39. [39]
  S. Jiang, H. Wan, H. Liu, et al., Appl. Phys. Lett. 109 (2016) 102904. doi: 10.1063/1.4962489
40. [40]
  W. Guo, C. Tan, K. Shi, et al., Nanoscale 10 (2018) 17751–17760. doi: 10.1039/c8nr05292a
41. [41]
  F. Chen, M. Jing, H. Yang, et al., Ionics 27 (2021) 1101–1111. doi: 10.1007/s11581-020-03891-0
42. [42]
  J. Jiang, A. Wang, W. Wang, et al., J. Energy Chem. 46 (2020) 114–122. doi: 10.1016/j.jechem.2019.10.009
1. [1]
  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
2. [2]
  Ziling Jiang , Shaoqing Chen , Chaochao Wei , Ziqi Zhang , Zhongkai Wu , Qiyue Luo , Liang Ming , Long Zhang , Chuang Yu . Enabling superior electrochemical performance of NCA cathode in Li_5.5PS_4.5Cl_1.5-based solid-state batteries with a dual-electrolyte layer. Chinese Chemical Letters, 2024, 35(4): 108561-. doi: 10.1016/j.cclet.2023.108561
3. [3]
  Haowen Li , Hongying Hou , Dai-Huo Liu , Bao Li , Dongmei Dai , Bao Wang , Mengmin Jia , Zhuangzhuang Zhang , Liang Wang , Yaru Qiao , Canhui Wu , Huihui Zhu , Pengyao Yan . A designed flexible solid-state electrolyte with rich hydrogen-bonded networks from TPU-PEGDA/LLZTO for Li metal batteries. Chinese Chemical Letters, 2026, 37(2): 111020-. doi: 10.1016/j.cclet.2025.111020
4. [4]
  Lisi Xu , Maosheng Li , Anqi He , Haijiao Xie , Kuirong Deng . F/N interface engineering of nonflammable polymer electrolyte for wide-temperature quasi-solid-state Li metal batteries. Chinese Chemical Letters, 2026, 37(2): 111815-. doi: 10.1016/j.cclet.2025.111815
5. [5]
  Ying Li , Yanjun Xu , Xingqi Han , Di Han , Xuesong Wu , Xinlong Wang , Zhongmin Su . A new metal–organic rotaxane framework for enhanced ion conductivity of solid-state electrolyte in lithium-metal batteries. Chinese Chemical Letters, 2024, 35(9): 109189-. doi: 10.1016/j.cclet.2023.109189
6. [6]
  Qianqian Song , Yunting Zhang , Jianli Liang , Si Liu , Jian Zhu , Xingbin Yan . Boron nitride nanofibers enhanced composite PEO-based solid-state polymer electrolytes for lithium metal batteries. Chinese Chemical Letters, 2024, 35(6): 108797-. doi: 10.1016/j.cclet.2023.108797
7. [7]
  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
8. [8]
  Biao Fang , Runwei Mo . PVDF-based solid-state battery. Chinese Journal of Structural Chemistry, 2024, 43(8): 100347-100347. doi: 10.1016/j.cjsc.2024.100347
9. [9]
  Bao Li , Pengyao Yan , Mengmin Jia , Liang Wang , Yaru Qiao , Haowen Li , Canhui Wu , Zhuangzhuang Zhang , Dongmei Dai , Dai-Huo Liu . Engineering lithiophilic LiC_x layer to robust interfacial chemistry between LAGP and Li anode for Li-metal batteries. Chinese Chemical Letters, 2025, 36(7): 110145-. doi: 10.1016/j.cclet.2024.110145
10. [10]
  Sheng Zhao , Junjie Lu , Bifu Sheng , Siying Zhang , Hao Li , Jizhang Chen , Xiang Han . High-performance room temperature solid-state lithium battery enabled by PP-PVDF multilayer composite electrolyte. Chinese Chemical Letters, 2025, 36(6): 110008-. doi: 10.1016/j.cclet.2024.110008
11. [11]
  Zhangran Ye , Zhixuan Yu , Jingming Yao , Lei Deng , Yunna Guo , Hantao Cui , Chongchong Ma , Chao Tai , Liqiang Zhang , Lingyun Zhu , Peng Jia . An ionically conductive and compressible sulfochloride solid-state electrolyte for stable all-solid-state lithium-based batteries. Chinese Chemical Letters, 2025, 36(8): 110272-. doi: 10.1016/j.cclet.2024.110272
12. [12]
  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
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]
  Jian Wang , Baohui Wang , Pin Ma , Yifei Zhang , Honghong Gong , Biyun Peng , Sen Liang , Yunchuan Xie , Hailong Wang . Regulation of uniformity and electric field distribution achieved highly energy storage performance in PVDF-based nanocomposites via continuous gradient structure. Chinese Chemical Letters, 2025, 36(4): 109714-. doi: 10.1016/j.cclet.2024.109714
15. [15]
  Yue Zheng , Tianpeng Huang , Pengxian Han , Jun Ma , Guanglei Cui . Cathodal Li-ion interfacial transport in sulfide-based all-solid-state batteries: Challenges and improvement strategies. Chinese Journal of Structural Chemistry, 2024, 43(10): 100390-100390. doi: 10.1016/j.cjsc.2024.100390
16. [16]
  Zi-Hao Zuo , Jiang-Kui Hu , Xi-Long Wang , Shi-Jie Yang , Wei-Qi Mai , Yao-Hui Zhu , Zheng Liao , Jia Liu , Hong Yuan , Jia-Qi Huang . Oxygen defect-mediated Li-ion transport for long-cycle solid-state lithium metal batteries. Chinese Chemical Letters, 2026, 37(5): 110851-. doi: 10.1016/j.cclet.2025.110851
17. [17]
  Xu Li , Yue Zhao , Tingli Ma . Improved polymer electrolyte interfacial contact via constructing vertically aligned fillers. Chinese Journal of Structural Chemistry, 2025, 44(2): 100406-100406. doi: 10.1016/j.cjsc.2024.100406
18. [18]
  Min Chen , Boyu Peng , Xuyun Guo , Ye Zhu , Hanying Li . Polyethylene interfacial dielectric layer for organic semiconductor single crystal based field-effect transistors. Chinese Chemical Letters, 2024, 35(4): 109051-. doi: 10.1016/j.cclet.2023.109051
19. [19]
  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
20. [20]
  Ziling Jiang , Chen Liu , Jie Yang , Xia Li , Chaochao Wei , Qiyue Luo , Zhongkai Wu , Lin Li , Liping Li , Shijie Cheng , Chuang Yu . Designing F-doped Li₃InCl₆ electrolyte with enhanced stability for all-solid-state lithium batteries in a wide voltage window. Chinese Chemical Letters, 2025, 36(6): 109741-. doi: 10.1016/j.cclet.2024.109741

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