Applications of polymer electrolytes in lithium batteries are lagged by the low ionic conductivity and lithium-ion transference number, and polymer electrolytes are mechanically weak to suppress lithium dendrites. Herein, two-dimensional layer-double-hydroxide (2D LDH) nanosheets are introduced into polyethylene oxide (PEO) as fillers for the first time. After blending with 2D LDH fillers, the composite polymer electrolyte (CPE) exhibits an optimized conductivity with a lithium-ion transference number of 0.42. Additionally, the mechanical strength and electrochemical stability of the CPE at high voltages are improved. More importantly, the CPE shows a markedly enhanced stability against dendritic lithium, and the current density for dendrite-free Li plating/stripping in the CPE arises to 800 μA cm⁻² at 60 °C. Solid-state lithium batteries based on the PEO/LDH CPEs show an initial discharge capacity of ~138 mA h g⁻¹ with a capacity retention of 88% after 100 cycles at 0.2 C and 60 °C.

低离子电导率和锂离子转移数使聚合物电解质在锂电池中的应用滞后，并且聚合物电解质在机械上较弱，无法抑制锂枝晶。在此，二维层双氢氧化物（2D LDH）纳米片首次引入聚环氧乙烷（PEO）中作为填充剂。与二维LDH填料共混后，复合聚合物电解质（CPE）表现出最佳的电导率，锂离子转移数为0.42。另外，提高了CPE在高压下的机械强度和电化学稳定性。更重要的是，CPE表现出对树枝状锂的显着增强的稳定性，并且CPE中无枝晶锂镀覆/剥离的电流密度达到800μAcm ^-2在60°C。基于PEO / LDH CPE的固态锂电池在0.2 C和60°C循环100次后，初始放电容量约为138 mA h g ^-1，容量保持率为88％。