High Partial Molar Volume Polymer Electrolyte for Upgraded Lithium Metal Batteries
Lithium (Li) metal batteries combined with solid electrolytes represent a highly promising technology for high-energy-density storage systems. However, their cycling performance encounters inferior stability due to the continuous growth of Li-dendrites. The initial motivation for Li-dendrite growth theoretically arises from the high chemical potential difference (∆µ) at the electrolyte/Li metal interface, yet the effectiveness of ∆µ regulation lacks experimental validation. Here, we experimentally present the impact of ∆µ on the growth of Li-dendrites through manipulation of the partial molar volume of Li<sup>+</sup> ( <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:semantics><mml:msub><mml:mi>V</mml:mi> <mml:msup><mml:mi>Li</mml:mi> <mml:mo>+</mml:mo></mml:msup> </mml:msub> <mml:annotation>${V}_{{\mathrm{Li}}^ + }$</mml:annotation></mml:semantics> </mml:math> ) in the polymer electrolyte. By weakening Li-O coordination structure, the as-produced high- <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:semantics><mml:msub><mml:mi>V</mml:mi> <mml:msup><mml:mi>Li</mml:mi> <mml:mo>+</mml:mo></mml:msup> </mml:msub> <mml:annotation>${V}_{{\mathrm{Li}}^ + }$</mml:annotation></mml:semantics> </mml:math> polymer electrolyte (108.5 cm<sup>3</sup> mol<sup>-1</sup>) shows 83% decrease in ∆µ (289 J mol<sup>-1</sup>) compared with conventional counterparts, thereby enabling stable cycling for >10 months in a Li||Li cell and >2000 cycles in a Li||Cu cell with an average Coulombic efficiency (CE) of 96%. To one's delight, a practical cylindrical Li||Li[Ni<sub>0.5</sub>Co<sub>0.3</sub>Mn<sub>0.2</sub>]O<sub>2</sub> cell with capacity of 0.62 Ah delivers excellent cycle stability with negligible capacity attenuation over 85 cycles at 0.2 C. The beneficial role of high <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:semantics><mml:msub><mml:mi>V</mml:mi> <mml:msup><mml:mi>Li</mml:mi> <mml:mo>+</mml:mo></mml:msup> </mml:msub> <mml:annotation>${V}_{{\mathrm{Li}}^ + }$</mml:annotation></mml:semantics> </mml:math> is leveraged to introduce a new dimension in polymer electrolyte engineering, highlighting the underexplored design strategy of regulating interfacial ∆µ to rejuvenate practical lithium metal batteries.
Authors
- Genqiang Zhang (ORCID: https://orcid.org/0000-0003-4887-536X)
- Xianfu Wang (ORCID: https://orcid.org/0000-0002-2066-7473)
- Shuyin Wang
- He Miao (ORCID: https://orcid.org/0000-0002-0250-913X)
- Tianyu Lei (ORCID: https://orcid.org/0009-0005-7009-2427)
- Dongjiang Chen (ORCID: https://orcid.org/0000-0002-0567-0850)
- Yin Hu (ORCID: https://orcid.org/0000-0003-3868-026X)
- Wei Chen (ORCID: https://orcid.org/0000-0002-1135-7721)
- Bowen Zhang (ORCID: https://orcid.org/0000-0002-3581-9476)
- Yichao Yan (ORCID: https://orcid.org/0000-0001-7889-6394)
- Yuxin Fan (ORCID: https://orcid.org/0000-0003-1561-1472)
- Yuanpeng Liu (ORCID: https://orcid.org/0000-0003-3099-3325)
- Mingjie Zhou (ORCID: https://orcid.org/0000-0002-4023-5811)
Institutions
- University of Science and Technology of China (CN)
- University of Electronic Science and Technology of China (CN)
- Harbin Institute of Technology (CN)
- National Engineering Research Center of Electromagnetic Radiation Control Materials (CN)
- State Key Laboratory of Electronic Thin Films and Integrated Devices
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-04-09
- DOI
- https://doi.org/10.1002/anie.202500896
- Citations
- 8
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 5.84