Pressure-tailored lithium deposition and dissolution in lithium metal batteries

Unregulated lithium (Li) growth is the major cause of low Coulombic efficiency, short cycle life and safety hazards for rechargeable Li metal batteries. Strategies that aim to achieve large granular Li deposits have been extensively explored, and yet it remains a challenge to achieve the ideal Li deposits, which consist of large Li particles that are seamlessly packed on the electrode and can be reversibly deposited and stripped. Here we report a dense Li deposition (99.49% electrode density) with an ideal columnar structure that is achieved by controlling the uniaxial stack pressure during battery operation. Using multiscale characterization and simulation, we elucidate the critical role of stack pressure on Li nucleation, growth and dissolution processes and propose a Li-reservoir-testing protocol to maintain the ideal Li morphology during extended cycling. The precise manipulation of Li deposition and dissolution is a critical step to enable fast charging and a low-temperature operation for Li metal batteries. Li electrodeposition is a fundamental process in Li metal batteries and its reversibility is crucial for battery operation. The authors investigate the effects of stack pressure on Li deposition and associated processes and discuss strategies for achieving dense Li deposits and practical Li metal batteries.