An Automated Electrochemistry Platform for Studying pH-dependent Molecular Electrocatalysis

Abstract

Comprehensive studies of molecular electrocatalysis require tedious titration-type experiments that slow down manual experimentation. We present elab as an automated electrochemical platform designed for molecular electrochemistry that uses opensource software to modularly interconnect various commercial instruments, enabling users to chain together multiple instruments for complex electrochemical operations. We benchmarked the solution handling performance of our platform through gravimetric calibration, acid-base titrations, and voltammetric diffusion coefficient measurements. We then used the platform to explore the TEMPO-catalyzed electrooxidation of alcohols, demonstrating our platforms capabilities for pH-dependent molecular electrocatalysis. We performed combined acid-base titrations and cyclic voltammetry on six different alcohol substrates, collecting 684 voltammograms with 171 different solution conditions over the course of 16 hours, demonstrating high throughput in an unsupervised experiment. The high versatility, transferability, and ease of implementation of elab promises the rapid discovery and characterization of pH-dependent processes, including mediated electrocatalysis for energy conversion, fuel valorization, and bioelectrochemical sensing, among many applications.