Smart gel polymer electrolytes enlightening high safety and long life sodium ion batteries
The overall performance of sodium-ion batteries, particularly regarding safety and cycle life, remains below expectations due to severe degradation of electrode materials and the electrode/electrolyte interphase. Herein, we develop a smart gel polymer electrolyte for hard carbon||NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> batteries through the in situ radical polymerization of a cyanoethylurea-containing methacrylate monomer and an isocyanate-based methacrylate monomer in conventional NaPF<sub>6</sub>-carbonate-based electrolytes. We demonstrate that the smart gel polymer electrolyte facilitates the formation of robust electrode/electrolyte interphase layers, thus improving the thermal and chem-electrochemical stability of the electrodes. When the temperature exceeds 120 °C, the in situ formed gel polymer electrolyte undergoes further crosslinking through nucleophilic addition reactions between urea and isocyanate motifs. This additional crosslinking blocks ion transportation and inhibits crosstalk effects, thus boosting the safety of pouch-type hard carbon||NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> batteries. Moreover, the smart gel polymer electrolyte enables hard carbon||NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> full cells to achieve improved cycle life even at the elevated temperature of 50 °C. The design philosophy behind the development of in situ formed smart gel polymer electrolytes offers valuable guidance for creating high-safety, long-life, and sustainable sodium-ion batteries.
Authors
- Zhiwei Hu (ORCID: https://orcid.org/0000-0003-0324-2227)
- Shanmu Dong (ORCID: https://orcid.org/0000-0002-2493-3556)
- Chuanchuan Li (ORCID: https://orcid.org/0000-0001-5891-6335)
- André Hilger (ORCID: https://orcid.org/0000-0002-6454-7967)
- Chien‐Te Chen (ORCID: https://orcid.org/0000-0002-1881-2600)
- Ingo Manke (ORCID: https://orcid.org/0000-0001-9795-5345)
- Xiangchun Zhuang
- Jun Ma (ORCID: https://orcid.org/0000-0001-5016-8096)
- Lang Huang (ORCID: https://orcid.org/0000-0002-6728-9510)
- Shenghang Zhang
- Jiedong Li (ORCID: https://orcid.org/0000-0001-9016-9042)
- Jingwen Zhao (ORCID: https://orcid.org/0000-0002-8695-159X)
- Huanrui Zhang (ORCID: https://orcid.org/0000-0002-9766-7607)
- Jiangwei Ju (ORCID: https://orcid.org/0000-0002-4391-7957)
- Guanglei Cui (ORCID: https://orcid.org/0000-0001-5987-7569)
- Fu Sun (ORCID: https://orcid.org/0000-0001-6787-6988)
- Tiantian Dong
- Bin Xie (ORCID: https://orcid.org/0000-0002-7247-1237)
- Yuhan Zhang (ORCID: https://orcid.org/0000-0003-4054-2552)
- Chenghao Sun (ORCID: https://orcid.org/0000-0001-5819-5582)
- Jinzhi Wang (ORCID: https://orcid.org/0000-0001-8696-377X)
- Fan-Hsiu Chang
- Li Du (ORCID: https://orcid.org/0009-0003-6284-4612)
- Chang‐Yang Kuo
- Gaojie J. Xu (ORCID: https://orcid.org/0000-0001-8810-7061)
Institutions
- National Yang Ming Chiao Tung University (TW)
- Helmholtz-Zentrum Berlin für Materialien und Energie (DE)
- National Synchrotron Radiation Research Center (TW)
- Max Planck Institute for Chemical Physics of Solids (DE)
- Qinghai New Energy (China) (CN)
- Marine Biomedical Research Institute of Qingdao (CN)
- Qingdao Institute of Bioenergy and Bioprocess Technology (CN)
- Qingdao Center of Resource Chemistry and New Materials (CN)
- Shandong University of Science and Technology (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-03-26
- DOI
- https://doi.org/10.1038/s41467-025-57964-7
- Citations
- 43
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 31.41
Funders
- National Natural Science Foundation of China
- Natural Science Foundation of Shandong Province