Liao Daniel W, Zeng Davy, Mulla Muzamil, Madanchi Ali, Kawakami Hiroki, Aihara Yuichi, Aotani Koichiro, Thouless M D, Dasgupta Neil P
Department of Mechanical Engineering, University of Michigan, Ann Arbor, MI, 48109, USA.
Department of Materials Science and Engineering, University of Michigan, Ann Arbor, MI, 48109, USA.
Adv Mater. 2025 Jul;37(29):e2502114. doi: 10.1002/adma.202502114. Epub 2025 May 12.
Carbon interlayers have been implemented in "anode-free" solid-state batteries to improve the uniformity and reversibility of lithium deposition by controlling the location of Li plating. However, there remains a lack of fundamental understanding of the detailed role of how these interlayers function during in situ Li formation. In this study, the relationships between the interfacial adhesion of the carbon interlayer to the solid electrolyte and the location of Li plating are investigated. By varying the lamination pressure used during manufacturing, the ability to systematically tune the resulting interfacial adhesion is demonstrated. Mechanical peel tests are performed, and a 4-fold increase in interfacial toughness is measured as the lamination pressure increases from 100 to 400 MPa. Post-mortem electron microscopy revealed that the location of Li plating with respect to the carbon interlayer transitions from the interface with the solid electrolyte to the current collector above a threshold interfacial toughness, which is consistent when the interlayer material is changed from amorphous to hard carbon. These findings highlight the role of electro-chemo-mechanical relationships in systematically controlling Li deposition in solid-state batteries when interlayers are present.
碳夹层已被应用于“无阳极”固态电池中，通过控制锂电镀的位置来提高锂沉积的均匀性和可逆性。然而，对于这些夹层在原位锂形成过程中如何发挥作用的详细机制，仍缺乏基本的了解。在本研究中，研究了碳夹层与固体电解质之间的界面附着力与锂电镀位置之间的关系。通过改变制造过程中使用的层压压力，展示了系统调节所得界面附着力的能力。进行了机械剥离试验，当层压压力从100 MPa增加到400 MPa时，测得界面韧性增加了4倍。死后电子显微镜显示，当界面韧性高于阈值时，相对于碳夹层的锂电镀位置从与固体电解质的界面转变为集流体，当夹层材料从非晶碳变为硬碳时，这一现象是一致的。这些发现突出了电化学-机械关系在存在夹层时系统控制固态电池中锂沉积的作用。
