CatPath‐GPT: A Mixture of Experts System for Computational Catalyst Design

ABSTRACT Despite advances in computational catalysis, the complexity of theoretical calculations and specialised expertise requirements limit the broader adoption of catalyst design tools. This work introduces CatPath‐GPT, a mixture‐of‐experts framework that democratizes computational catalyst design by integrating three AI specialists: product prediction (77.2% accuracy), computational planning, and automated code generation through a unified BERT‐based router. Experimental validation through two case studies demonstrates practical impact: systematic screening of Cu x Zn 1 − x catalysts identifies optimal compositions for selective CO 2 RR (Cu 75 Zn 25 for ethanol), while high‐throughput metal oxide screening reproduces Nørskov's classical scaling relationships and identifies high‐activity materials. Benchmarking against GPT‐4 and Mistral‐7B demonstrates superior performance across catalyst‐related tasks, particularly in modeling complex surface reactions. The open‐source framework enables researchers without computational expertise to perform advanced catalyst design, potentially transforming how catalytic materials are discovered and optimized.