Machine-learning rationalization and prediction of solid-state synthesis conditions

TL;DR

This paper presents a machine-learning approach that predicts solid-state synthesis conditions from large datasets, revealing key factors like precursor stability and extending existing rules to oxide systems, aiding experimental design.

Contribution

The study introduces a novel machine-learning framework that accurately predicts synthesis conditions and uncovers underlying factors influencing solid-state reactions, expanding understanding beyond traditional thermodynamic considerations.

Findings

Optimal heating temperatures correlate with precursor stability.

Reaction thermodynamics are less predictive of synthesis conditions.

Machine-learning models achieve good predictive performance.

Abstract

There currently exist no quantitative methods to determine the appropriate conditions for solid-state synthesis. This not only hinders the experimental realization of novel materials but also complicates the interpretation and understanding of solid-state reaction mechanisms. Here, we demonstrate a machine-learning approach that predicts synthesis conditions using large solid-state synthesis datasets text-mined from scientific journal articles. Using feature importance ranking analysis, we discovered that optimal heating temperatures have strong correlations with the stability of precursor materials quantified using melting points and formation energies ($\Delta G_f$, $\Delta H_f$). In contrast, features derived from the thermodynamics of synthesis-related reactions did not directly correlate to the chosen heating temperatures. This correlation between optimal solid-state heating temperature and precursor stability extends Tamman's rule from intermetallics to oxide systems, suggesting the importance of reaction kinetics in determining synthesis conditions. Heating times are shown to be strongly correlated with the chosen experimental procedures and instrument setups, which may be indicative of human bias in the dataset. Using these predictive features, we constructed machine-learning models with good performance and general applicability to predict the conditions required to synthesize diverse chemical systems. Codes and data used in this work can be found at: https://github.com/CederGroupHub/s4.