At-Scale Discovery of High-Voltage Cathode Active Materials for Na-Ion Batteries via Charged-Only Structures and Committee Divide-and-Conquer Learning
Year: 2026
Type: preprint
Abstract: Current cathode-active materials (CAMs) designed for sodium-ion batteries (SIBs) suffer from low operating voltages, limited energy density, irreversible phase transitions, and low intrinsic electrical conductivity. In this work, we have developed generalizable and transferable descriptor-based machine learning (ML) models, along with composition- and graph-based neural networks (NNs) and transfer learning (TL) models, all trained on a dataset of charged-only structures rather than charged/discharged pairs. Using a committee of the top four trained ML models, the mean voltage is predicted as the target property. More importantly, we show that uncertainty quantification can improve the reliability of candidate selection for training subsequent higher-generation models by including structures for which the current committee models are least confident. In this way, the new expensive ab initio data provide information in regions where the original models most need improvement. We have showcased the transferability of the final generation models by applying them to a large database of Na-free inorganic host structures curated from Materials Project, AFLOW, OQMD, and GNoME for at-scale SIB CAM discovery. A comprehensive interactive online database, NaCAM-Atlas, was also developed, containing 14,843 CAMs with voltages greater than 3 V for SIBs. Finally, a subset of the top-ranked candidate CAMs was validated through explicit, high-throughput first-principles calculations of voltage profiles, structural robustness upon sodiation/desodiation, and electronic properties. Together, this integrated data curation, ML training and improvement, and first-principles validation strategy establishes a scalable and transferable framework for accelerating the discovery of stable, high-voltage CAMs for SIBs and beyond.
Source: arXiv (Cornell University)
Institution: University of Missouri–Kansas City
Language: English
Subfield: Materials Chemistry
Field: Materials Science
Domain: Physical Sciences
Open Access status: green
Funder: National Science Foundation
Awards: Track 4: Advanced CI Coordination Ecosystem: Monitoring and Measurement Services, Track 1: ACCESS Resource Allocations Marketplace and Platform Services (RAMPS), ACO: An Open CI Ecosystem to Advance Scientific Discovery (OpenCI), Track 3: COre National Ecosystem for CyberinfrasTructure (CONECT), Track 2: Customized Multi-tier Assistance, Training, and Computational Help (MATCH) for End User ACCESS to CI
OpenAlex ID: W7162553240