Autonomous experiments were conducted using our previously developed eLab platform in combination with BO. In brief, eLab uses opensource software to modularly interconnect a potentiostat to solution handling hardware and other peripheral instruments, enabling users to chain together multiple operations to carry out complex electrochemical experiments. A carbonate/bicarbonate buffer (pH 9.8) was selected to maintain optimal conditions for TEMPO catalysis, and a glassy carbon electrode, which is inactive towards the direct oxidation of alcohols, was used as the working electrode. Experimental parameters, including Ccat (1-6 mM), Csub (1-300 mM), and ν (5 mV/s-5 V/s), were constrained based on practical considerations. CVs were measured by sweeping from 0 V to 0.9 V vs. Ag/AgCl and back.