Cross-Linked PVA/HNT Composite Separator Enables Stable Lithium-Organic Batteries under Elevated Temperature

Li-organic batteries (LOBs) are promising advanced battery systems because of their unique advantages in capacity, cost, and sustainability. However, the shuttling effect of soluble organic redox intermediates and the intrinsic dissolution of small-molecular electrodes have hindered the practical application of these cells, especially under high operating temperatures. Herein, a cross-linked membrane with abundant negative charge for high-temperature LOBs is prepared via electrospinning of poly(vinyl alcohol) containing halloysite nanotubes (HNTs). The translocation of negatively charged organic intermediates can be suppressed by the electronic repulsion and the cross-linked network while the positively charged Li⁺ are maintained, which is attributed to the intrinsic electronegativity of HNTs and their well-organized and homogeneous distribution in the PVA matrix. A battery using a PVA/HNT composite separator (EPH-10) and an anthraquinone (AQ) cathode exhibits a high initial discharge capacity of 231.6 mAh g^-1 and an excellent cycling performance (91.4% capacity retention, 300 cycles) at 25 °C. Even at high temperatures (60 and 80 °C), its capacity retention is more than 89.2 and 80.4% after 100 cycles, respectively. Our approach demonstrates the potential of the EPH-10 composite membrane as a separator for high-temperature LOB applications.