Rectifying interphases for preventing Li dendrite propagation in solid-state electrolytes
Rectifying interphases for preventing Li dendrite propagation in solid-state electrolytes
复制标题
纠正界面以防止固态电解质中锂枝晶的生长
DOI：
10.1039/d2ee04006a
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发表时间：
2023
影响因子：
32.5
通讯作者：
Yao X
中科院分区：
文献类型：
--
作者：
Yao X
固态电解液已经成为安全和高能量锂金属电池的基石，但仍然面临着锂树枝晶生长和界面不相容的严峻挑战。本工作采用界面工程的方法，在固体电解质和锂金属阳极之间引入了电子整流界面。整流行为抑制了电子向电解液的渗透，从而有效地减少了枝晶。这种界面相由p-Si/n-TiO2结和外部铝层组成，采用多步溅射沉积技术在石榴石颗粒表面形成。通过片上器件的不对称I-V响应研究了电子整流行为，并通过颗粒上的电子电导测量进一步证实了电子整流行为的一个数量级的低电流响应。Al层有助于界面的相容性，这从亲锂表面和降低的界面阻抗得到了验证。通过锂对称电池的电化学测量表明，寿命从几十个小时显著提高到两个月以上。用X射线计算机层析技术重建了固态电解液的三维形貌，观察到了Li枝晶扩展行为的减少。
Solid-state electrolytes have emerged as the grail for safe and energy-dense Li metal batteries but still face significant challenges of Li dendrite propagation and interfacial incompatibility. In this work, an interface engineering approach is applied to introduce an electronic rectifying interphase between the solid-state electrolyte and Li metal anode. The rectifying behaviour restrains electron infiltration into the electrolyte, resulting in effective dendrite reduction. This interphase consists of a p-Si/n-TiO2 junction and an external Al layer, created using a multi-step sputter deposition technique on the surface of garnet pellets. The electronic rectifying behaviour is investigated via the asymmetric I–V responses of on-chip devices and further confirmed via the one-order of magnitude lower current response by electronic conductivity measurements on the pellets. The Al layer contributes to interface compatibility, which is verified from the lithiophilic surface and reduced interfacial impedance. Electrochemical measurements via Li symmetric cells show a significantly improved lifetime from dozens of hours to over two months. The reduction of the Li dendrite propagation behaviour is observed through 3D reconstructed morphologies of the solid-state electrolyte by X-ray computed tomography.