Efficient Pourbaix diagrams of many-element compounds

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• Pourbaix diagrams are crucial for predicting material stability in aqueous electrochemical systems.
• Current methods struggle with complex, multi-component materials due to high computational costs.
• High-throughput material discovery necessitates more efficient stability analysis tools.

Purpose of the Study:

• To develop a computationally efficient method for constructing Pourbaix diagrams for complex multicomponent systems.
• To address the limitations of existing Pourbaix analysis algorithms for systems with four or more elements.
• To enable broader application of Pourbaix analysis in materials discovery and electrochemical engineering.

Main Methods:

• Proposed an alternative Pourbaix construction algorithm filtering species to the compositional convex hull.
• Incorporated axes for H+ and e- quantities to ensure inclusion of all stable phase mixtures.
• Integrated the new algorithm into pymatgen and the Materials Project.

Main Results:

• Reduced computational time for Pourbaix diagram construction by several orders of magnitude.
• Successfully applied the method to complex multicomponent systems.
• Enabled accurate stability predictions for previously intractable systems.

Conclusions:

• The new convex hull-based Pourbaix algorithm significantly enhances computational efficiency.
• This advancement facilitates the stability analysis of complex materials for electrochemical applications.
• The method is now accessible via pymatgen and the Materials Project, supporting materials research.