AI-guided high-throughput discovery of iridium- and ruthenium-free palladium-oxide catalysts for durable acidic oxygen evolution

Original abstract

Catalyzing acidic oxygen evolution at the proton-exchange-membrane water electrolysis (PEMWE) anode relies almost entirely on iridium or ruthenium, drawn from concentrated supply chains that constrain gigawatt-scale deployment. We report an artificial intelligence (AI)-guided, human-supervised closed-loop platform (>90% automation) integrating combinatorial sputter synthesis, high-throughput screening, machine-learning composition-property models, adaptive multi-objective optimization, and context-aware large-language-model reasoning, where lead catalysts advanced to long-term validation in 1 M H2SO4 at 10 mA cm-2. Navigating a combinatorial metal oxide space, the platform iteratively evaluated the activity-stability trade-off of 2,942 catalysts across 53 material systems and 26 elements, surfacing Ir- and Ru-free complex oxides such as InMnPdOx and NiTaPdOx that conventional design logic, and off-the-shelf language models, would not predict. In retrospective benchmarking, our sequential learning agent advanced the activity-stability frontier faster than fixed-policy Bayesian optimization or in-context language-model selection. During long-term testing, NiTaPdOx operated at lower overpotential than PdOx, but both eventually exceeded 0.5 V: PdOx at ~200 h and NiTaPdOx at ~470 h. InMnPdOx showed a similar overpotential improvement in addition to a dramatic increase in operational stability, retaining overpotential below 0.5 V over 1,000 h of operation. The additive elements promote the formation of a nanostructure that is associated with catalytic activity while stabilizing Pd against corrosion. The results highlight the power of AI-driven science in addressing long-standing challenges in materials chemistry, and the greater availability of Pd relative to incumbent Ir and Ru offers a near-term option to ease supply constraints on scaled electrochemical H2 generation.