Tuning of dynamic solvation structures via click chemistry for PEO-based solid polymer electrolytes

Ruiyang Li¹, Xueying Yang², Qichen Chen¹, Boyang Huang³, Siyu Zhao⁴, Peng Zhang⁵, Jie Lin⁶, Jinbao Zhao^{7

8}

Affiliations

¹ College of Chemistry and Chemical Engineering, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technology, Ministry of Education, Collaborative Innovation Center of Chemistry for Energy Materials, Xiamen University, Xiamen, 361005, China.
² College of Energy, Xiamen University, Xiamen, 361102, China.
³ Anhui Provincial Key Laboratory of Advanced Catalysis and Energy Materials, Ultra High Molecular Weight Polyethylene Fiber Engineering Research Center of Anhui Province, Anqing Normal University, Anqing, 246133, China.
⁴ Department of Engineering Science, University of Oxford, Oxford, OX1 3PJ, UK.
⁵ College of Energy, Xiamen University, Xiamen, 361102, China. pengzhang@xmu.edu.cn.
⁶ School of Mechanical and Aerospace Engineering, Queen's University Belfast, Belfast, BT9 5AH, UK. j.lin@qub.ac.uk.
⁷ College of Chemistry and Chemical Engineering, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technology, Ministry of Education, Collaborative Innovation Center of Chemistry for Energy Materials, Xiamen University, Xiamen, 361005, China. jbzhao@xmu.edu.cn.
⁸ College of Energy, Xiamen University, Xiamen, 361102, China. jbzhao@xmu.edu.cn.

PMID: 41038845
DOI: 10.1038/s41598-025-16709-8

Tuning of dynamic solvation structures via click chemistry for PEO-based solid polymer electrolytes

Ruiyang Li et al. Sci Rep. 2025.

. 2025 Oct 2;15(1):34332.

doi: 10.1038/s41598-025-16709-8.

Authors

Ruiyang Li¹, Xueying Yang², Qichen Chen¹, Boyang Huang³, Siyu Zhao⁴, Peng Zhang⁵, Jie Lin⁶, Jinbao Zhao^{7

8}

Affiliations

¹ College of Chemistry and Chemical Engineering, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technology, Ministry of Education, Collaborative Innovation Center of Chemistry for Energy Materials, Xiamen University, Xiamen, 361005, China.
² College of Energy, Xiamen University, Xiamen, 361102, China.
³ Anhui Provincial Key Laboratory of Advanced Catalysis and Energy Materials, Ultra High Molecular Weight Polyethylene Fiber Engineering Research Center of Anhui Province, Anqing Normal University, Anqing, 246133, China.
⁴ Department of Engineering Science, University of Oxford, Oxford, OX1 3PJ, UK.
⁵ College of Energy, Xiamen University, Xiamen, 361102, China. pengzhang@xmu.edu.cn.
⁶ School of Mechanical and Aerospace Engineering, Queen's University Belfast, Belfast, BT9 5AH, UK. j.lin@qub.ac.uk.
⁷ College of Chemistry and Chemical Engineering, State-Province Joint Engineering Laboratory of Power Source Technology for New Energy Vehicle, State Key Laboratory of Physical Chemistry of Solid Surfaces, Engineering Research Center of Electrochemical Technology, Ministry of Education, Collaborative Innovation Center of Chemistry for Energy Materials, Xiamen University, Xiamen, 361005, China. jbzhao@xmu.edu.cn.
⁸ College of Energy, Xiamen University, Xiamen, 361102, China. jbzhao@xmu.edu.cn.

PMID: 41038845
DOI: 10.1038/s41598-025-16709-8

Abstract

The Li⁺-transport mechanisms in both solid polymer electrolytes (SPEs) and liquid electrolytes (LEs) are fundamentally governed by solvation dynamics, requiring an optimal balance between continuous coordination and moderate binding strength. Poly(ethylene oxide) (PEO) is a classic SPE matrix that leverages its -CH₂-CH₂-O- (EO) segments to provide continuous oxygen coordination for Li⁺ transport via amorphous regions. While continuous EO segments facilitate the intra-chain Li⁺-transport, their strong multidentate solvation of Li⁺ through a chelate effect - each Li⁺ chelates with 4-6 ethylene oxide (EO) units - significantly hinders the inter-chain Li⁺ mobility. This effect creates rigid solvation cages that both immobilize Li⁺ and resist modification by alternative moieties (e.g. carbonate or nitrile groups), resulting in poor room-temperature ionic conductivity (σ) and low Li⁺ transference number (t_Li+). To address these challenges, we developed a series of precise Li⁺-transport models (LTMs) through click chemistry, strategically combining acrylate-PEG and acrylonitrile to engineer balanced interactions between multidentate (EO) and monodentate (C = O, C ≡ N) coordination sites. This design achieved synergistic enhancement of both inter- and intra-chain transport pathways, demonstrated by significantly improved performance with σ = 6.40 × 10^{- 5} S/cm and t_Li+ = 0.44 at 25 °C. This approach permits tailored control of dynamic solvation structures, offering new opportunities to enhance Li⁺ transport in PEO-based solid polymer electrolytes.

Keywords: Click chemistry; Li+ transport; Lithium-ion batteries; Poly(ethylene oxide); Solid polymer electrolyte.

PubMed Disclaimer

Conflict of interest statement

Competing interests: The authors declare no competing interests.

References

1. Lee, M. J. et al. Elastomeric electrolytes for high-energy solid-state lithium batteries. Nature 601, 217–222. https://doi.org/10.1038/s41586-021-04209-4 (2022). - DOI - PubMed
1. Armand, M. & Tarascon, J. M. Building better batteries. Nature 451, 652–657. https://doi.org/10.1038/451652a (2008). - DOI - PubMed
1. Popovic, J. Dry polymer electrolyte concepts for Solid-State batteries. Macromol. Chem. Phys. 223, 96. https://doi.org/10.1002/macp.202100344 (2021).
1. Yu, X., Xue, L., Goodenough, J. B. & Manthiram, A. Ambient-Temperature All-Solid-State sodium batteries with a laminated composite electrolyte. Adv. Funct. Mater. 31, 523. https://doi.org/10.1002/adfm.202002144 (2021).
1. Jung, Y. C. et al. Room-temperature performance of poly(ethylene ether carbonate)-based solid polymer electrolytes for all-solid-state lithium batteries. Sci. Rep. 7, 526. https://doi.org/10.1038/s41598-017-17697-0 (2017).

Save citation to file

Email citation

Add to Collections

Add to My Bibliography

Your saved search

Create a file for external citation management software

Your RSS Feed

Tuning of dynamic solvation structures via click chemistry for PEO-based solid polymer electrolytes

Affiliations

Tuning of dynamic solvation structures via click chemistry for PEO-based solid polymer electrolytes

Authors

Affiliations

Abstract

Conflict of interest statement

References

Grants and funding