ARCADE: Automated and Interpretable Design of Complex Catalysts

Abstract The rational design of high-performance catalysts is pivotal for modern industry but is often hindered by the time-consuming nature of trial-and-error methods. While computational and data-driven approaches have accelerated materials discovery, significant challenges remain, especially for complex systems like multielement disordered nanoparticles. These challenges include immense computational costs, difficulties in modeling stability and heterogeneous active sites, and a lack of interpretability in “black-box” AI models. To address these multifaceted challenges, herein, we introduce ARCADE (Automated Rational Catalyst Design), a generalizable and transferable framework for the automated and interpretable design of complex catalysts. This highly cohesive pipeline introduces key methodological innovations in realistic structure generation, autonomous active-site processing, and short-range order guided interpretability, seamlessly coupled with state-of-the-art pH-dependent microkinetic modeling. Notably, ARCADE streamlines the structural modeling of irregular nanoparticles by transforming intractable combinatorial enumeration into a targeted iterative search; robustly identifies active sites and subsequently resolves ubiquitous adsorbate drift issues arising during structural relaxations; and employs geometric short-range order descriptors derived contribution scores to rapidly decode catalytic mechanisms, thereby efficiently unraveling the complex synergistic effects inherent in multielement catalysts. Using the challenging design of multielement nanoparticle catalysts for CO2 reduction reaction (CO2RR) as a representative system, we demonstrate that ARCADE can systematically navigate the design process, from evaluating material stability to identifying site-specific activity and selectivity. Our results show that this methodology substantially accelerates the development cycle for complex catalysts, confirming its feasibility and broad applicability. Crucially, this work establishes a fully integrated paradigm for the rational design and discovery of complex materials for challenging chemical reactions.