Abstract:We demonstrate the fabrication of graphene liquid marbles as photothermal miniature reactors with precise temperature control for reaction kinetics modulation. Graphene liquid marbles show rapid and highly reproducible photothermal behavior while maintaining their excellent mechanical robustness.B yt uning the applied laser power, swift regulation of graphene liquid marbles surface temperature between 21-135 8 8Ca nd its encapsulated water temperature between 21-74 8 8Ca re demonstrated. The temperature regulation modulates the reaction kinetics in our graphene liquid marble,a chieving a1 2-fold superior reaction rate constant for methylene blue degradation than at room temperature.Liquid marbles are formed by the spontaneous encapsulation of liquid droplets by pulverized solid particles.[1] They are promising miniature reactors owing to their ability to isolate microliter liquid, ease of fabrication, and excellent mechanical robustness.[2] Such miniature reactor is ideal for reactions involving costly and hazardous reagents/processes,and useful in preliminary reaction screening. Liquid marble reactors have been applied for blood typing, [3] nanocomposite synthesis, [4] photochemical polymerization, [5] and heterogeneous catalysis.[6] However,c urrent applications of liquid marble reactors are restricted to reactions of low activation energy or at room temperature due to the lack of aheating mechanism. It is essential to incorporate aheating mechanism into liquid marble to broaden its application for reactions requiring precise control and elevated temperature.Graphene is ap romising candidate for heatable liquid marble miniature reactor due to their excellent photothermal properties.[7] Their strong photoabsorption over awide range of wavelengths allows rapid and localized heating upon vibrational relaxation of photoexcited electrons.[8] Currently, the incorporation of graphene are mainly in the form of suspensions or films, [9] which require tedious reactant/product recovery procedures,a nd/or film fabrication protocols. Hence,t he combination of graphene and liquid marble allows easy-to-prepare heatable miniature reactor,a nd permits abroad range of processes with precise temperature and reaction kinetic control. Notably,the localized photothermal heating is crucial as thermal energy is supplied to the smallvolume reaction on-demand without changing the bulk liquid medium temperature.[10] This reduces the evaporation issues of miniature reactors and minimizes energy waste,m aking it superior to conduction/convection heating. [10] Herein, we demonstrate the fabrication of graphene liquid marbles (GLM) and their application as remotely heatable miniature reactors for reaction kinetic modulation. The physical and mechanical properties of GLM as isolated and robust miniature reactors are characterized. We then demonstrate the instant heating of GLM with surface temperatures tunable between 21 to 135 8 8Cb yc ontrolling the laser power. Theactual encapsulated water temperature is probed using temperature-d...