Long-term space missions require extra-terrestrial production of storable, renewable energy. Hydrogen is ascribed a crucial role for transportation, electrical power and oxygen generation. We demonstrate in a series of drop tower experiments that efficient direct hydrogen production can be realized photoelectrochemically in microgravity environment, providing an alternative route to existing life support technologies for space travel. The photoelectrochemical cell consists of an integrated catalyst-functionalized semiconductor system that generates hydrogen with current densities >15 mA/cm2 in the absence of buoyancy. Conditions are described adverting the resulting formation of ion transport blocking froth layers on the photoelectrodes. The current limiting factors were overcome by controlling the micro- and nanotopography of the Rh electrocatalyst using shadow nanosphere lithography. The behaviour of the applied system in terrestrial and microgravity environment is simulated using a kinetic transport model. Differences observed for varied catalyst topography are elucidated, enabling future photoelectrode designs for use in reduced gravity environments.
Photoelectrochemical devices integrate the processes of light absorption, charge separation, and catalysis for chemical synthesis. The monolithic design is interesting for space applications, where weight and volume constraints predominate. Hindered gas bubble desorption and the lack of macroconvection processes in reduced gravitation, however, limit its application in space. Physico‐chemical modifications of the electrode surface are required to induce gas bubble desorption and ensure continuous device operation. A detailed investigation of the electrocatalyst nanostructure design for light‐assisted hydrogen production in microgravity environment is described. p‐InP coated with a rhodium (Rh) electrocatalyst layer fabricated by shadow nanosphere lithography is used as a model device. Rh is deposited via physical vapor deposition (PVD) or photoelectrodeposition through a mask of polystyrene (PS) particles. It is observed that the PS sphere size and electrocatalyst deposition technique alter the electrode surface wettability significantly, controlling hydrogen gas bubble detachment and photocurrent–voltage characteristics. The highest, most stable current density of 37.8 mA cm−2 is achieved by depositing Rh via PVD through 784 nm sized PS particles. The increased hydrophilicity of the photoelectrode results in small gas bubble contact angles and weak frictional forces at the solid–gas interface which cause enhanced gas bubble detachment and enhanced device efficiency.
Photoelectrochemical (PEC) cells offer the possibility of carbon-neutral solar fuel production through artificial photosynthesis. The pursued design involves technologically advanced III-V semiconductor absorbers coupled via an interfacial film to an electrocatalyst layer. These systems have been prepared by in situ surface transformations in electrochemical environments. High activity nanostructured electrocatalysts are required for an efficiently operating cell, optimized in their optical and electrical properties. We demonstrate that shadow nanosphere lithography (SNL) is an auspicious tool to systematically create three-dimensional electrocatalyst nanostructures on the semiconductor photoelectrode through controlling their morphology and optical properties. First results are demonstrated by means of the photoelectrochemical production of hydrogen on p-type InP photocathodes where hitherto applied photoelectrodeposition and SNL-deposited Rh electrocatalysts are compared based on their J-V and spectroscopic behavior. We show that smaller polystyrene particle masks achieve higher defect nanostructures of rhodium on the photoelectrode which leads to a higher catalytic activity and larger short circuit currents. Structural analyses including HRSEM and the analysis of the photoelectrode surface composition by using photoelectron spectroscopy support and complement the photoelectrochemical observations. The optical performance is further compared to theoretical models of the nanostructured photoelectrodes on light scattering and propagation.
Electrochemical energy conversion technologies play a crucial role in space missions, for example, in the Environmental Control and Life Support System (ECLSS) on the International Space Station (ISS). They are also vitally important for future long-term space travel for oxygen, fuel and chemical production, where a re-supply of resources from Earth is not possible. Here, we provide an overview of currently existing electrolytic energy conversion technologies for space applications such as proton exchange membrane (PEM) and alkaline electrolyzer systems. We discuss the governing interfacial processes in these devices influenced by reduced gravitation and provide an outlook on future applications of electrolysis systems in, e.g., in-situ resource utilization (ISRU) technologies. A perspective of computational modelling to predict the impact of the reduced gravitational environment on governing electrochemical processes is also discussed and experimental suggestions to better understand efficiency-impacting processes such as gas bubble formation and detachment in reduced gravitational environments are outlined.
The absence of strong buoyancy forces severely complicates the management of multiphase flows in microgravity. Different types of space systems, ranging from in-space propulsion to life support, are negatively impacted by this effect. Multiple approaches have been developed to achieve phase separation in microgravity, whereas they usually lack the robustness, efficiency, or stability that is desirable in most applications. Complementary to existing methods, the use of magnetic polarization has been recently proposed to passively induce phase separation in electrolytic cells and other two-phase flow devices. This article illustrates the dia- and paramagnetic phase separation mechanism on MilliQ water, an aqueous MnSO4 solution, lysogeny broth, and olive oil using air bubbles in a series of drop tower experiments. Expressions for the magnetic terminal bubble velocity are derived and validated and several wall–bubble and multi-bubble magnetic interactions are reported. Ultimately, the analysis demonstrates the feasibility of the dia- and paramagnetic phase separation approach, providing a key advancement for the development of future space systems.
Efficient artificial photosynthesis systems are currently realized as catalyst- and surface-functionalized photovoltaic tandem and triple junction devices [1,2] enabling photoelectrochemical water oxidation while simultaneously recycling CO2 and generating hydrogen as a solar fuel for storable renewable energy. The successful implementation of an efficient photoelectrochemical (PEC) water splitting cell is not only a highly desirable approach to solving the energy challenge on earth: an effective air revitalization system generating a constant flux of O2 while simultaneously recycling CO2 and providing a sustainable fuel supply is also essential for the International Space Station and long-term space missions, where a regular resupply from earth is not possible. We recently demonstrated in a series of drop tower experiments that efficient direct hydrogen production can be realized photoelectrochemically in microgravity environment, providing an alternative route to existing life support technologies for space travel [3]. Current limiting factors such as the absence of macroconvection processes were overcome by controlling the micro- and nanotopography of the electrocatalyst using shadow nanosphere lithography (SNL), generating so-called catalytic ‘hot-spots’ on the electrode surface which prevent gas bubble coalescence [3,4]. We found that the J-V characteristics of the half-cell and the overall device efficiency in microgravity environment are significantly affected by alterations in the electrocatalyst nanotopography [5]. By varying the shape and distance of catalytic ‘hot-spots’ on the electrode surface, we could control the gas bubble radius upon detachment from the electrode surface and the light absorption properties of the semiconductor in free fall. Shadow nanosphere lithography can therefore be used as a prosperous tool to develop custom-tailored electrocatalyst nanostructures of high fidelity on a light-absorbing semiconductor surface for an optimized device performance in microgravity and terrestrial applications. [1] Young J. L., Steiner M. A., Döscher H., France R. M., Turner J. A., Deutsch T. G. (2017). “Direct solar-to-hydrogen conversion via inverted metamorphic multi-junction semiconductor architectures”, Nat. Energ. 2. (17028). [2] Cheng W. H., Richter M. H., May M. M., Ohlmann J., Lackner D., Dimroth F., Hannappel T., Atwater H. A., Lewerenz H. J (2018). “Monolithic Photoelectrochemical Device for 19% Direct Water Splitting”, ACS Energy Lett. 3, 8, 1795-1800. [3] Brinkert K., Richter M. H., Akay Ö., Liedtke J., Gierisig M., Fountaine K. T., Lewerenz H. J. (2018). Efficient Solar Hydrogen Production in Microgravity Environment. Nat. Commun. 9 (2527). [4] Patoka P., Giersig M. (2011). “Self-assembly of latex particles for the creation of nanostructures with tunable plasmonic properties”, J. Mater. Chem. 21, 16783-16796. [5] Brinkert K., Richter M. H., Akay Ö., Giersig M., Fountaine K. T., Lewerenz H.-J. (2018). “Advancing semiconductor-electrocatalyst systems: application of surface transformation films and nanosphere lithography”, Faraday Discuss. 208, 523-535.
Artificial photosynthesis systems, which follow the concept of the Z-scheme of natural photosynthesis, are presently being realized as catalyst-functionalized photovoltaic tandem devices for the photoelectrochemical oxidation of water and the simultaneous generation of hydrogen as a so-called “solar fuel”. The successful implementation of an efficient photoelectrochemical (PEC) water splitting cell is not only a highly desirable approach to solving the energy challenge on earth: an effective air revitalization system generating a constant flux of O2 while simultaneously recycling CO2 and providing a sustainable fuel supply is also essential for the International Space Station and long-term space missions, where a regular resupply from earth is not possible. Here, we present the photoelectrochemical production of hydrogen in microgravity environments on p-type indium phosphide electrodes with deposited rhodium electrocatalysts. Our findings indicate that microgravity has a significant impact on the gas bubble evolution behaviour and the mass transfer rate of the evolved hydrogen gas on the electrode surface. Furthermore, microgravity influences the current-voltage characteristics and the overall solar-to-hydrogen efficiency of the catalyst functionalized semiconductor-based half-cell. Further experiments with nanostructured rhodium catalysts fabricated by shadow nanosphere lithography on the InP surface suggest that the structure of the electrode surface plays a significant role for the gas bubble evolution behaviour and for the further the development of efficient prototypes for solar-assisted water splitting and hydrogen production that operate in micro- and hypergravity environments.
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