Electrocatalysis is poised to play a pivotal role in future energy material and chemical manufacturing. The rational design of next-generation electrocatalysts - guided by sound scientific hypothesis - is essential for advancing practical technologies. In recent years, my team at Argonne has actively explored high-performance electrocatalysts using innovative design and synthesis strategies. In this presentation, I will first discuss our recent advances in utilizing metal–organic frameworks (MOFs) as tunable precursors for oxygen redox electrocatalysis. This includes the development of platinum-group-metal-free (PGM-free) and ultralow-platinum catalysts for proton exchange membrane fuel cells [1], as well as PGM-free catalysts as viable replacements for iridium for water electrolysis [2]. I will then introduce our recent studies on the selective electrochemical reduction of CO₂ to multi-carbon (C₂⁺) products, where the reaction pathways and product distributions are profoundly modulated by active-site geometry, atomic coordination, and nanoconfinement effects [3–5].
The presentation outlines our integrated approach that combines advanced structural and spectroscopic characterization, computational modeling, and machine-learning-guided discovery to uncover catalytic mechanisms and guide materials optimization. Finally, I will discuss the implications of these findings for the scalable design of next-generation electrocatalysts in future energy conversion and storage applications.
[1] “Ultralow-loading platinum-cobalt fuel cell catalysts derived from imidazolate frameworks” L. Chong, et. al. Science 362, 1276–1281 (2018)
[2] “La- and Mn-doped cobalt spinel oxygen evolution catalyst for proton exchange membrane electrolysis” L. Chong, et. al. Science 380, 609–616 (2023)
[3] “Highly selective electrocatalytic CO2 reduction to ethanol by metallic clusters dynamically formed from atomically dispersed copper” H. Xu, et. al. Nature Energy, 5, 623–632 (2020)
[4] “Modulating CO2 electrocatalytic conversion to organics pathway by the catalytic site dimension”, H. Xu, J. Am. Chem. Soc., 146, 10357−10366, (2024)
[5] “Direct Electrochemical Reduction of CO2 to C2+ Chemicals: Catalysts, Microenvironments, and Mechanistic Understanding” S. Guo, et. al. ACS Energy Letter, 10, 600−619 (2025)