Discovering new stable mayenite-like electrides using high-throughput computational screening
Abstract
Electrides are an emerging class of materials presenting electrons in off-nuclei pockets and exceptional properties. Since the discovery of the first inorganic electride (Ca12Al14O32-2e-, mayenite), many new electrides have emerged. Notably, while most electrides are unstable in air and moisture sensitive, mayenite can be used in uncontrolled atmosphere at room temperature without degradation. We hypothesize that the unique stability of mayenite comes from the way it is made. Most electrides are directly synthesized by solid-state synthesis in controlled environment. On the other hand, mayenite is made by forming a highly stable non-electride Ca12Al14O33 that is treated by a reducing agent (e.g., Ti) that will selectively remove oxygen forming Ca12Al14O32-2e-. This selective deintercalation approach or soft-chemistry synthesis route is likely to form electrides that are (meta-)stable in air. The goal of this project is to use computational screening to search for mayenite-like electrides that could be made by soft-chemistry approaches. Using high-throughput computations, we will browse the wavefunction obtained from Density Functional Theory (DFT) for thousands of known inorganic materials. We will select materials that show unoccupied electron states that have an off-nuclei nature and in a second step evaluate if anions can be selectively removed or cations can be added to fill this electride state. After this screening, we will identify a series of possible new electrides that we will further study in terms of refined electronic structure, work function and thermoionic emission. Beyond the identification of new electrides, the data generated will offer opportunities in understanding what structural and chemical factors favor electrides formation. Our work will also advance materials science beyond electrides as soft-chemistry approaches has grown in importance in many other fields (e.g., recent nickelates unconventional superconductors).
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Feb 06, 2025
- Source ID
- FA95502410095
Entities
People
- Geoffroy Hautier
Organizations
- Air Force Office of Scientific Research
- Board of Trustees of Dartmouth College
- United States Air Force