Active Learning Driven Materials Discovery for Low Thermal Conductivity Rare-Earth Pyrochlore for Thermal Barrier Coatings

TL;DR

This study employs an active learning framework with Bayesian optimization and a random forest model to efficiently discover rare-earth pyrochlore materials with low thermal conductivity suitable for thermal barrier coatings.

Contribution

It introduces an active learning approach combining Bayesian optimization and machine learning to accelerate the discovery of complex pyrochlore materials with desired thermal properties.

Findings

Successfully identified two pyrochlore compositions with low thermal conductivity.

The surrogate model accurately predicted thermal conductivity for new compositions.

Synthesis revealed phase formation issues, indicating areas for model improvement.

Abstract

High-Entropy/multicomponent rare-earth oxides (HECs and MCCs) show promise as alternative materials for thermal barrier coatings (TBC) with the ability to tailor properties based on the combination of rare-earth elements present. By enabling the substitution of scarce or supply-risk rare-earths with more readily available alternatives while maintaining comparable material performance, HECs and MCCs offer a valuable path towards alternative TBC material design. However, navigating this search space of compositionally complex materials is both time and resource intensive. In this study, an active learning (AL) framework was employed to identify HEC/MCC materials with a pyrochlore structure, with acceptable thermal conductivity (TC) for TBC applications. The AL framework was applied through a Bayesian optimisation (BO) strategy, coupled with a random forest surrogate model. TC was selected as the optimisation criterion as that is the most basic requirement of TBC materials. Over two iterations of the AL cycle, four compositions were generated and synthesized in the lab for experimental evaluation. The first iteration yielded two single-phase pyrochlores, $(La_{0.29}Nd_{0.36}Gd_{0.36})_2Zr_2O_7$ and $(La_{0.333}Nd_{0.26}Gd_{0.15}Ho_{0.15}Yb_{0.111})_2Zr_2O_7$, with measured thermal conductivities of 2.03 and 1.90 $W/mK$, respectively. The surrogate model predicted a TC of 2.009 $W/mK$ for both compositions, demonstrating it's accuracy for completely new compositions. The second iteration compositions showed dual-phase when synthesized, highlighting the need to take into account phase formation in the AL framework.