eRoboChem: Autonomous Electrosynthesis Across Redox Modes and Reactor Designs

Synthetic electrochemistry offers powerful opportunities for molecular synthesis, yet its broader adoption remains hindered by the complexity of electrochemical reaction development. Beyond conventional reaction parameters, electrosynthesis requires careful choice of electrode materials, reactor designs and control of electron transfer, creating a complex experimental and optimisation challenge that can deter many synthetic chemists. Here, we introduce eRoboChem, a modular self-driving laboratory that integrates automated experimentation, analytical feedback and Bayesian optimisation across complementary flow and batch electrochemical reactors. Its versatility is demonstrated through three transformations spanning paired, oxidative and reductive electrosynthesis, each presenting distinct experimental challenges. Fully closed-loop flow operation enables autonomous reaction optimisation while accommodating gas evolution, whereas a complementary human-in-the-loop high-throughput batch module addresses electrode passivation and facilitates electrode screening. Systematic comparisons with conventional optimisation strategies, including one-factor-at-a-time and design of experiments approaches, demonstrate the value of Bayesian optimisation for navigating complex reaction spaces and extracting chemically meaningful and complementary insights. By adapting the experimental architecture to the requirements of the chemistry, rather than constraining the chemistry to a fixed reactor design, eRoboChem establishes a flexible framework for autonomous electrosynthesis and represents a step towards making electrochemical methodologies more accessible to the broader synthetic community.