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Autonomous laboratories can accelerate discoveries in chemical synthesis, but this requires automated measurements coupled with reliable decision-making 1 , 2 . Most autonomous laboratories involve bespoke automated equipment 3 – 6 , and reaction outcomes are often assessed using a single, hard-wired characterization technique 7 . Any decision-making algorithms 8 must then operate using this narrow range of characterization data 9 , 10 . By contrast, manual experiments tend to draw on a wider range of instruments to characterize reaction products, and decisions are rarely taken based on one measurement alone. Here we show that a synthesis laboratory can be integrated into an autonomous laboratory by using mobile robots 11 – 13 that operate equipment and make decisions in a human-like way. Our modular workflow combines mobile robots, an automated synthesis platform, a liquid chromatography–mass spectrometer and a benchtop nuclear magnetic resonance spectrometer. This allows robots to share existing laboratory equipment with human researchers without monopolizing it or requiring extensive redesign. A heuristic decision-maker processes the orthogonal measurement data, selecting successful reactions to take forward and automatically checking the reproducibility of any screening hits. We exemplify this approach in the three areas of structural diversification chemistry, supramolecular host–guest chemistry and photochemical synthesis. This strategy is particularly suited to exploratory chemistry that can yield multiple potential products, as for supramolecular assemblies, where we also extend the method to an autonomous function assay by evaluating host–guest binding properties. A modular autonomous platform for general exploratory synthetic chemistry uses mobile robots to integrate an automated synthesis platform and two analysis platforms.

The resurgence of photocatalysis has propelled the development of a variety of novel synthetic reactions powered by visible light. However, the majority of photocatalysts typically used in these reactions are homogenous dyes or expensive organometallic complexes, which have issues with cost, and recyclability which hinders large-scale applications. The following work first summarizes the recent developments in modern photoredox catalysis, along with some advances in high throughput experiments. This thesis then describes the use of a high-throughput screening strategy to discover a covalent triazine framework, CTF-2, as heterogeneous organic photocatalyst for a variety of reactions, including conjugate addition, metallaphotoredox arylation, metallaphotoredox alkylation, dehydrogenative arylation, and fluorination. Finally, progress towards a fully-autonomous workflow for photochemical reaction optimization using mobile robots is highlighted.