Chen Ya, Yao Liu, Chen Xiaodong, Jin Jun, Wu Meifen, Wang Qing, Zha Wenping, Wen Zhaoyin
CAS Key Laboratory of Materials for Energy Conversion, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, P. R. China.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Science, Beijing 100049, P. R. China.
ACS Appl Mater Interfaces. 2022 Mar 9;14(9):11950-11961. doi: 10.1021/acsami.1c24506. Epub 2022 Feb 22.
Sulfide-type solid electrolytes (SSEs) are supposed to be preferential candidates for all-solid-state Li metal batteries (ASSLMBs) due to their satisfactory Li conductivity and preferable mechanical stiffness. Nonetheless, the poor stability between the Li anode and SSEs and uncontrolled Li dendrite growth severely restrict their commercial application. Herein, an amphiphilic LiSiO-enriched solid electrolyte interphase (SEI) as a "Janus" layer was first introduced at the Li/SSEs interface, and it exhibited bond coupling reactivity with both the Li anode and SSEs by forming Li-S, Li-O-Si, and Si-S covalent bonds, which is called the pincer effect. In addition to the physical isolation of Li and SSEs to prevent side reactions between them, LiSiO with high ionic conductivity offers abundant and evenly distributed transport channels for fast Li migration. As evidenced by in situ microscopy, the high-strength anodic interface constructed by the pincer effect and in situ decomposition mentioned above is free from mechanical damage during the Li plating/stripping. As a result, the symmetric cells exert an outstanding cycling performance for over 2000 h at 0.2 mA cm and even 500 h at 0.5 mA cm without evident resistance growth. The artificial SEI layer with the pincer effect and its effective application in interfacial stabilization put forward a new perspective for the commercialization of ASSLMBs.
硫化物型固体电解质（SSEs）因其令人满意的锂导电性和较好的机械刚度，被认为是全固态锂金属电池（ASSLMBs）的优先候选材料。然而，锂负极与SSEs之间稳定性差以及锂枝晶生长不受控制，严重限制了它们的商业应用。在此，一种富含两性LiSiO的固体电解质界面（SEI）作为“两面神”层首次被引入到锂/SSEs界面，它通过形成Li-S、Li-O-Si和Si-S共价键，与锂负极和SSEs都表现出键耦合反应性，这被称为钳位效应。除了对锂和SSEs进行物理隔离以防止它们之间的副反应外，具有高离子导电性的LiSiO为快速的锂迁移提供了丰富且分布均匀的传输通道。原位显微镜观察表明，由上述钳位效应和原位分解构建的高强度阳极界面在锂电镀/剥离过程中没有机械损伤。因此，对称电池在0.2 mA cm下表现出超过2000 h的出色循环性能，在0.5 mA cm下甚至能循环500 h且没有明显的电阻增长。具有钳位效应的人工SEI层及其在界面稳定化方面的有效应用为ASSLMBs的商业化提出了一个新的视角。
