Thermodynamics of Sodium-Lead Alloys for Negative Electrodes from First-Principles

Lee, D. K. J.; Deng, Z.; Gautam, G. S.; Canepa, P.

doi:10.1021/acs.chemmater.4c00592

Thermodynamics of Sodium-Lead Alloys for Negative Electrodes from First-Principles

D. K. J. Lee, Z. Deng, G. S. Gautam, and P. Canepa; Chem. Mater. 36, 6831 (2024).

C. N. R. Rao at 90

BibTeX

@article{Lee2024thermodynamics,
  author  = {Lee, D. K. J. and Deng, Z. and Gautam, G. S. and Canepa, P.},
  title   = {{Thermodynamics of Sodium-Lead Alloys for Negative Electrodes from First-Principles}},
  journal = {Chemistry of Materials},
  volume  = {36},
  pages   = {6831},
  year    = {2024},
  doi     = {10.1021/acs.chemmater.4c00592}
}

Brief summary

Lead is one of the most recycled metals, making it a candidate for cheap, high-capacity anodes in sodium-ion batteries. We compute the phase diagram of sodium–lead alloys and their alloying voltages, clarify the boundaries of key phases, and find that their strongly ordered compounds leave no room for solid solutions at intermediate and high sodium contents.

Full abstract

Metals, such as tin, antimony, and lead (Pb) have garnered renewed attention for their potential use as alloyant-negative electrode materials in sodium (Na)-ion batteries (NIBs). Despite Pb’s toxicity and its high molecular weight, lead is one of the most commonly recycled metals, positioning Pb as a promising candidate for a cost-effective, high-capacity anode material. Understanding the miscibility of Na into Pb is crucial for the development of high-energy density negative electrode materials for NIBs. Using a first-principles multiscale approach, we analyze the thermodynamic properties and estimate the Na-alloying voltage of the Na-Pb system by constructing the compositional phase diagram. In the Na-Pb system, we elucidate the phase boundaries of important phases, such as Pb-rich face-centered cubic and β-NaPb₃, thereby improving our understanding of the phase diagram of the Na-Pb alloy. Due to the strong ordering tendencies of the Na-Pb intermetallics (such as NaPb, Na₅Pb₂, and Na₁₅Pb₄), we do not observe any solid-solution behavior at intermediate and high Na concentrations.