Thermodynamic Understanding of Li-Dendrite Formation

The recent boom in electrical energy storage and conversion with high-energy density facilitates the exploration of Li-metal batteries. However, Li dissolution and nucleation are easily susceptible to thermodynamic conditions that induce dendrite growth, causing tremendous safety hazards, low energy density, and short lifespan. Nevertheless, a comprehensive understanding of the thermodynamic effects on lithium deposition and growth is still absent. The development and latest research progress of thermodynamic-inducing factors regarding lithium nucleation and growth are systematically summarized from theory to experiment, especially focusing on thermodynamic energy, temperature, and related models. Strategies for designing a dendrite-free Li-metal anode through thermodynamic considerations, including structured anode, self-healing dendrite tactics, and electrode and electrolyte interface engineering are also discussed. We highlight the imperfections of present thermodynamic research and propose corresponding feasible solutions. Future work should evaluate each individual system on its own to integrate suitable models that combine with kinetics and other factors to find interrelated strategies to address the dendrite-growth issues under various conditions.