Automated electrochemistry is emerging as a powerful tool to accelerate discoveries in important fields such as energy storage, catalysis, electrosynt…

There is a critical need for predictably modulating the reactivity of redox-active polymers (RAPs) to improve their performance in applications such as catalysis, energy storage, and sensing. However,...

Manganese dissolution has been a long-standing problem that limits the widespread application of Mn-based Li-ion battery (LIB) cathodes, despite their low cost and high Li storage capacity. The accura...

Molecular electrocatalysis campaigns often require tuning multiple experimental parameters to obtain kinetically insightful electrochemical measurements, a prohibitively time-consuming task when performing comprehensive studies across multiple catalysts and substrates. In this work, we present an autonomous workflow that combines Bayesian optimization and automated electrochemistry to perform fully unsupervised cyclic voltammetry (CV) studies of molecular electrocatalysis. We developed CV descriptors that leveraged the conceptual framework of the EC′ (where EC′ denotes an electrochemical step followed by a catalytic chemical step) kinetic zone diagram to enable efficient Bayesian optimization. The CV descriptor’s effect on optimization performance was evaluated using a digital twin of our autonomous experimental platform, quantifying the accuracy of obtained kinetic values against the known ground truth. We demonstrated our platform experimentally by performing autonomous studies of TEMPO-catalyzed ethanol and isopropanol electro-oxidation, demonstrating rapid identification of kinetically insightful conditions in 10 or less iterations through the closed-loop workflow. Overall, this work highlights the application of autonomous electrochemical platforms to accelerate mechanistic studies in molecular electrocatalysis and beyond.

Automated, rapid electrocatalyst discovery techniques that comprehensively address the exploration of chemical spaces, characterization of catalyst robustness, reproducibility, and translation of resu...

Current recycling paradigms of lead-acid batteries (LABs) involve the use of toxic, polluting, and energy-demanding processes. Here we report a novel …

Correlation Between Microscopic Current Fluctuations Observed at Ultra-Microelectrodes and Macroscopic Bulk Electrolysis Performance in Redox-Active Microemulsions, Armando Santiago-Carboney, Filip Konstantinov, Michael A. Pence, Brian Barth, Adam Imel, Thomas Zawodzinski, Joaquín Rodríguez-López