Strain Coupled (110)-Oriented Lithium Anodes for High-Rate and High-Capacity Epitaxial Growth

Abstract Lithium metal is considered as the ultimate anode for high-energy-density batteries, yet its practical realization is thwarted by dendrite proliferation and chemomechanical interfacial instability. While epitaxial growth on crystallographically textured substrates provides a template for ordered deposition, sustaining this ordered growth under high capacities and current densities remains a formidable kinetic challenge. Herein, we overcome this barrier by engineering an elastic (110)-oriented lithium anode (e-Li (110)) comprising a conductive polymer scaffold. The e-Li (110) integrates preferred (110) crystallographic orientation with a mechanically coupled strain corresponding to the optimized 4% tensile-strain condition. Consequently, this strain-engineering strategy enables a capacity of 30 mAh cm–2 and current density of 25 mA cm–2 before lithium epitaxial breakdown. 5.9 Ah Li || LiNi0.8Co0.1Mn0.1O2 (NCM811) pouch cells with a high energy density of 509.8 Wh kg–1 show 90% capacity retention after 140 cycles. In sulfide-based all-solid-state batteries (ASSBs), e-Li (110) anode enables stable cycling for over 1600 cycles at a rate of 5 C. By highlighting strain as a critical parameter, our work provides a strategy for mechano-electrochemical coupling in lithium metal anodes for high-rate, high-energy-density batteries.