Commercial separators for lithium-ion batteries still have shortcomings such as inferior electrolyte wettability, serious thermal shrinkage (polyolefin separators) and intrinsic brittleness (ceramic separators), which result in poor electrochemical performance and serious potential safety hazard. Here, a waterborne separator is fabricated by deposition and in situ crosslinking of a homogeneous aqueous suspension containing natural clay nanorods (attapulgite, ATP) and polyvinylalcohol (PVA) onto both the external and internal surfaces of the Celgard^@2400 matrix. Different from conventional grafted or coated functional separators, the ATP-PVA/Celgard separator has a unique sandwiching/infusing structure. The separator features super-electrolyte-philicity with a liquid electrolyte contact angle of 0°, high Li⁺ conductivity (0.782 mS cm⁻¹), excellent mechanical properties and high thermostability. Consequently, the 4.9 V Li/LiNi_0.5Mn_1.5O₄ cell with the separator shows higher cycling stability (94.7% after 100 cycles), better rate performance and lower resistance than the cell with commercial ceramic separator. Moreover, the separator could improve performance of the Li/LiFePO₄ cell and stable open circuit voltage at 160 °C. This work provides an avenue for the design of advanced separators for high-voltage lithium-ion batteries via an environmentally friendly method using natural nanomaterials.

商用的锂离子电池隔膜仍然具有诸如电解液润湿性差，热收缩严重（聚烯烃隔膜）和固有脆性（陶瓷隔膜）等缺点，这导致电化学性能差和严重的潜在安全隐患。这里，水性分离器通过沉积和制造原位含有天然粘土纳米棒（绿坡缕石，ATP）和聚乙烯醇（PVA）到的Celgard的外部和内部表面的均匀含水悬浮液的交联^@2400矩阵。ATP-PVA / Celgard隔膜与传统的接枝或涂层功能隔膜不同，具有独特的夹心/灌注结构。该隔膜具有超电解质亲和性，液体电解质接触角为0°，具有高Li ⁺电导率（0.782 mS cm ^-1），优异的机械性能和高热稳定性。因此，与使用工业陶瓷隔板的电池相比，带有隔板的4.9 V Li / LiNi _0.5 Mn _1.5 O ₄电池显示出更高的循环稳定性（100次循环后为94.7％），更好的倍率性能和更低的电阻。此外，隔膜可以提高Li / LiFePO _4的性能电池和160°C的稳定开路电压。这项工作为通过使用天然纳米材料的环保方法设计用于高压锂离子电池的高级隔膜提供了途径。