John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA.
Nature. 2021 May;593(7858):218-222. doi: 10.1038/s41586-021-03486-3. Epub 2021 May 12.
A solid-state electrolyte is expected to suppress lithium (Li) dendrite penetration with high mechanical strength. However, in practice it still remains challenging to realise a lithium metal anode for batteries, because micrometre- or submicrometre-sized cracks in ceramic pellets can frequently be generated during battery assembly or long-time cycling. Once cracks form, lithium dendrite penetration is inevitable. Here we describe a solid-state battery design with a hierarchy of interface stabilities (to lithium metal responses), to achieve an ultrahigh current density with no lithium dendrite penetration. Our multilayer design has the structure of a less-stable electrolyte sandwiched between more-stable solid electrolytes, which prevents any lithium dendrite growth through well localized decompositions in the less stable electrolyte layer. A mechanism analogous to the expansion screw effect is proposed, whereby any cracks are filled by dynamically generated decompositions that are also well constrained, probably by the 'anchoring' effect the decompositions induce. The cycling performance of the lithium metal anode paired with a LiNiMnCoO cathode is very stable, with an 82 per cent capacity retention after 10,000 cycles at a 20C rate (8.6 milliamps per centimetre squared) and 81.3 per cent capacity retention after 2,000 cycles at a 1.5C rate (0.64 milliamps per centimetre squared). Our design also enables a specific power of 110.6 kilowatts per kilogram and specific energy up to 631.1 watt hours per kilogram at the micrometre-sized cathode material level.
固态电解质有望通过高机械强度抑制锂(Li)枝晶的穿透。然而,在实践中,要实现用于电池的锂金属阳极仍然具有挑战性,因为在电池组装或长时间循环过程中,陶瓷颗粒中经常会产生微米或亚微米大小的裂纹。一旦形成裂纹,锂枝晶的穿透是不可避免的。在这里,我们描述了一种具有界面稳定性层次(对锂金属的响应)的固态电池设计,以实现超高电流密度而不会出现锂枝晶穿透。我们的多层设计具有较不稳定电解质夹在较稳定固体电解质之间的结构,这可防止任何锂枝晶通过在较不稳定电解质层中局部分解而生长。提出了类似于膨胀螺钉效应的机制,其中任何裂纹都被动态生成的分解物填充,这些分解物也受到很好的限制,可能是由于分解物诱导的“锚固”效应。与 LiNiMnCoO 阴极配对的锂金属阳极的循环性能非常稳定,在 20C 速率(8.6 毫安厘米平方)下循环 10,000 次后容量保持率为 82%,在 1.5C 速率(0.64 毫安厘米平方)下循环 2,000 次后容量保持率为 81.3%。我们的设计还可以在微米级阴极材料水平上实现 110.6 千瓦每千克的比功率和高达 631.1 瓦时每千克的比能量。