The realisation of long-term space missions as well as lunar habitats require reliable and efficient oxygen and chemical producing devices e.g., for life support, fuel generation and in-situ resource utilisation (ISRU). We have recently demonstrated that integrated semiconductor-electrocatalyst systems can be operated in microgravity environments generated for 9.2 s at the Bremen Drop Tower (Center of Applied Space Technology and Microgravity, ZARM) at terrestrial efficiencies, thus opening the possibility of utilising these photoelectrochemical (PEC) devices for chemical synthesis in space. 1,2 , 3 Our findings reveal that by altering the electrocatalyst surface morphology through nanostructuring, we can introduce catalytic hot-spots on the photoelectrode which - through their hydrophilic nature - can also enhance gas bubble detachment in microgravity and thus circumvent the near-absence of buoyancy.1,3 We have found that the surface hydrophilicity and electrocatalyst loading require however careful balancing as the most effective nanostructures for gas bubble desorption can also result in less catalyst material on the photoelectrode surface, which in turn leads to a non-optimal PEC device performance.Here, we present a combined theoretical and experimental microfluidic, optical and photoelectrocatalytic performance analysis of photoelectrodes with integrated, nanostructured electrocatalysts, aiming at providing a guideline for an optimal design for microgravity applications. Focusing on the hydrogen evolution reaction (HER) and a well-investigated photoabsorber for this reaction, p-type InP, we firstly built an optoelectronic model in COMSOL Multiphysics in pursuit of quantifying the optical performance enhancements of Rh and Pt electrocatalyst nanostructures such as nanopyramids, nanowires and sub-wavelength aperture holes.4 We then developed a microfluidic model using the same nanostructure geometries to predict the hydrophilicity of the device surface and subsequently, the gas bubble contact angle. The best-performing nanostructured photoelectrodes predicted in our models where then manufactured, photoelectrochemically tested and fully optically and spectroscopically characterised. Predicted local electric field enhancements through catalytic hotspot formation were moreover experimentally validated using scanning electrochemical cell microscopy (SECCM). Our findings indicate that our developed optoelectronic and microfluidic models can be utilised to design a theoretical framework for identifying ideal electrocatalyst nanostructures for microgravity applications.References Brinkert K, et al. Efficient solar hydrogen generation in microgravity environment. Nature Communications 9, (2018). Brinkert K, Mandin P. Fundamentals and future applications of electrochemical energy conversion in space. npj Microgravity 8, (2022). Akay Ö, et al. Releasing the Bubbles: Nanotopographical Electrocatalyst Design for Efficient Photoelectrochemical Hydrogen Production in Microgravity Environment. Advanced Science 9, 2105380 (2022). Tembhurne S, Haussener S. Integrated Photo-Electrochemical Solar Fuel Generators under Concentrated Irradiation. Journal of The Electrochemical Society 163, H988 (2016). Pan Y, Huang S, Li F, Zhao X, Wang W. Coexistence of superhydrophilicity and superoleophobicity: theory, experiments and applications in oil/water separation. Journal of Materials Chemistry A 6, 15057-15063 (2018).