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).

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}
}

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.