Computational Screening of Current Collectors for Enabling Anode-Free Lithium Metal Batteries

Lithium metal cells are key for achieving high specific energy for electrification of transportation and aviation. Anode-free cells are lithium metal cells involving no excess lithium with the highest possible specific energy. In addition, anode-free cells are simpler, cheaper, and safer because they avoid the handling and manufacturing of lithium metal foils. The lack of excess lithium magnifies issues related to dendrite growth and poor cycling in anode-free cells. The electrolyte and current collector surface play a crucial role in affecting anode-free cell cycling performance. In this work, we have computationally screened for candidate current collectors that nucleate lithium effectively and allow uniform growth. These are determined by the free energy of lithium adsorption and lithium surface diffusion barrier on candidate current collectors. Using density functional theory calculations, we show that Li alloys possess ideal characteristics for Li nucleation and growth. These can lead to vastly improved performance compared to current transition-metal current collectors.