A Polyamide Gel Polymer Electrolyte Hybridizing SiO₂ Aerogel for High-Energy-Density Lithium Metal Batteries

TY - JOUR

T1 - A Polyamide Gel Polymer Electrolyte Hybridizing SiO2 Aerogel for High-Energy-Density Lithium Metal Batteries

AU - Zhang, Yuxiang

AU - Li, Zihan

AU - Zhang, Yuanxing

AU - Ma, Ming

AU - Wu, Yongchun

AU - Dai, Zhongjia

AU - Mu, Daobin

N1 - Publisher Copyright: © 2025 Wiley-VCH GmbH.

PY - 2026/2/6

Y1 - 2026/2/6

N2 - Lithium metal batteries (LMBs) hold immense promise for next-generation high-energy-density storage systems. However, inherent challenges including unstable solid electrolyte interphases (SEIs) and dendrite growth, critically impede its practical deployment in high-energy-density batteries. Herein, a composite poly(N,N'-Methylenebisacrylamide) (PMBA) gel polymer electrolyte hybridizing SiO2 aerogel (SiO2/PMBA GPE) is developed through in situ polymerization. The SiO2 aerogel incorporation accelerates Li+ transport by disrupting polymer chain alignment, and simultaneously regulates Li+ solvation structures through Lewis acid-base interactions between SiO2 aerogel and electrolyte components. This synergistic effect facilitates rapid kinetics and uniform Li deposition, as well as promotes a stable Li3N, LiF-rich interphase that may suppress dendrite growth. The SiO2/PMBA-based Li||Cu half-cell achieves a high average coulombic efficiency (CE) of 97.7% over 300 cycles after the initial activation stage at 0.1 mA cm−2, while Li||Li symmetrical cell demonstrates exceptional cycling stability exceeding 4000 h at 0.1 mA cm−2, indicating superior compatibility with lithium metal anode. The Li||NCM811 cell exhibits high discharge capacity of 171.6 mA g−1 at 1 C, and outstanding cycling stability with 90.6% capacity retention after 300 cycles. Noteworthy, the pouch cell with practical Li||NCM811 configuration achieves a high energy density of 453.87 Wh kg−1. The in situ polymerized SiO2/PMBA GPE design exhibits a promising prospect for the practical application of high energy density LMBs.

AB - Lithium metal batteries (LMBs) hold immense promise for next-generation high-energy-density storage systems. However, inherent challenges including unstable solid electrolyte interphases (SEIs) and dendrite growth, critically impede its practical deployment in high-energy-density batteries. Herein, a composite poly(N,N'-Methylenebisacrylamide) (PMBA) gel polymer electrolyte hybridizing SiO2 aerogel (SiO2/PMBA GPE) is developed through in situ polymerization. The SiO2 aerogel incorporation accelerates Li+ transport by disrupting polymer chain alignment, and simultaneously regulates Li+ solvation structures through Lewis acid-base interactions between SiO2 aerogel and electrolyte components. This synergistic effect facilitates rapid kinetics and uniform Li deposition, as well as promotes a stable Li3N, LiF-rich interphase that may suppress dendrite growth. The SiO2/PMBA-based Li||Cu half-cell achieves a high average coulombic efficiency (CE) of 97.7% over 300 cycles after the initial activation stage at 0.1 mA cm−2, while Li||Li symmetrical cell demonstrates exceptional cycling stability exceeding 4000 h at 0.1 mA cm−2, indicating superior compatibility with lithium metal anode. The Li||NCM811 cell exhibits high discharge capacity of 171.6 mA g−1 at 1 C, and outstanding cycling stability with 90.6% capacity retention after 300 cycles. Noteworthy, the pouch cell with practical Li||NCM811 configuration achieves a high energy density of 453.87 Wh kg−1. The in situ polymerized SiO2/PMBA GPE design exhibits a promising prospect for the practical application of high energy density LMBs.

KW - SiO aerogel

KW - gel polymer electrolytes (GPEs)

KW - high energy density

KW - in situ polymerization

KW - polyamide

UR - https://www.scopus.com/pages/publications/105025574933

U2 - 10.1002/smll.202512649

DO - 10.1002/smll.202512649

M3 - Article

AN - SCOPUS:105025574933

SN - 1613-6810

VL - 22

JO - Small

JF - Small

IS - 8

M1 - e12649

ER -