Poly(ethylene oxide) (PEO)‐based composite solid electrolytes (CSEs) are promising to accelerate commercialization of solid‐state lithium metal batteries (SSLMBs). Nonetheless, this is hindered by the CSEs' limited ion conductivity at room temperature. Here, we propose design, synthesis, and application of the bioinspired neuron‐like nanofillers for PEO‐based CSEs. The neuron‐like superhydrophobic nanofillers are synthesized by controllably grafting silicone nanofilaments onto montmorillonite nanosheets. Compared to various reported fillers, the nanofillers can greatly improve ionic conductivity (4.9 × 10−4 S cm−1, 30 °C), Li+ transference number (0.63), oxidation stability (5.3 V) and mechanical properties of the PEO‐based CSEs because of the following facts. The distinctive neuron‐like structure and the resulting synaptic‐like connections establish numerous long‐distance continuous channels over various directions in the PEO‐based CSEs for fast and uniform Li+ transport. Consequently, the assembled SSLMBs with the CSEs and LiFePO4 or NCM811 cathodes display superior cycling stability over a wide temperature range of 50 °C to 0 °C. Surprisingly, the pouch batteries with the large‐scale prepared CSEs kept working after being repeatedly bent, folded, cut or even punched in air. We believe that design of neuron‐like nanofillers is a viable approach to produce CSEs with high room temperature ionic conductivity for SSLMBs.

中文翻译：

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用于宽工作温度锂金属电池的类神经元硅酮纳米丝@蒙脱土纳米填料的PEO基固态电解质

聚环氧乙烷（PEO）基复合固体电解质（CSE）有望加速固态锂金属电池（SSLMB）的商业化。尽管如此，CSE 在室温下有限的离子电导率阻碍了这一点。在这里，我们提出了基于 PEO 的 CSE 的仿生神经元纳米填料的设计、合成和应用。通过将有机硅纳米丝可控地接枝到蒙脱土纳米片上来合成神经元样超疏水纳米填料。与各种报道的填料相比，纳米填料可以极大地提高PEO基材料的离子电导率（4.9 × 10−4 S cm−1，30 °C）、Li+迁移数（0.63）、氧化稳定性（5.3 V）和机械性能。 CSE 是因为以下事实。独特的类神经元结构和由此产生的类突触连接在基于 PEO 的 CSE 中的各个方向上建立了许多长距离连续通道，以实现快速、均匀的 Li+ 传输。因此，使用 CSE 和 LiFePO4 或 NCM811 阴极组装的 SSLMB 在 50 °C 至 0 °C 的宽温度范围内表现出卓越的循环稳定性。令人惊讶的是，采用大规模制备的CSE的软包电池在空气中反复弯曲、折叠、切割甚至冲压后仍能正常工作。我们相信，类神经元纳米填料的设计是为 SSLMB 生产具有高室温离子电导率的 CSE 的可行方法。