Navigating Ternary Doping in Li‐ion Cathodes With Closed‐Loop Multi‐Objective Bayesian Optimization

Abstract

ABSTRACT To further improve secondary battery materials, we are increasingly exploring highly complex composition spaces in attempts to optimize multiple properties simultaneously. While our past work has done this in systematic manners using high‐throughput experimentation, the exponential increase in the search space with triple doping makes grid search prohibitively expensive. Here, we demonstrate a closed‐loop, multi‐objective machine learning approach to guide the high‐throughput workflow to efficiently navigate a space with approximately 14 million unique combinations. The test system is LiCoPO 4 , which we have previously explored using systematic codoping that was effective in optimizing one property only: energy density. To learn multiple electrochemical metrics, we first pretrain a set transformer on the public Materials Project database as a feature extractor, then attach a multi‐task Gaussian process head and finetune the entire model on our high‐throughput data. Through 3 rounds of active learning, we demonstrate that with a very small number of samples (as few as 125 random compositions and 63 predicted), we are able to simultaneously optimize four key electrochemical properties. Relative to the undoped system, the best composition raises our composite figure of merit up to five times. This establishes an end‐to‐end workflow for accelerated battery materials design to be used in the rapidly growing field of autonomous materials discovery.