DMREF: INFEWS: Collaborative Research: Photocatalyst by Design: Computational Screening of Reconstructed Perovskite Semiconductor Electrodes for Efficient Solar-to-Fuel Conversion

Non-technical Abstract: The production of hydrogen fuel from sunlight and seawater has the potential to profoundly reshape the food-energy-water (FEW) landscape and to revolutionize the generation of electric power for transportation and residential applications. Hydrogen is a sustainable energy carrier whose catalytic reaction with oxygen generates electrical energy and heat without emitting carbon dioxide; the only byproduct of this reaction is clean water. Solar-to-hydrogen conversion offers the advantage of not requiring agricultural resources to produce synthetic fuels, overcoming one of the major constraints currently imposed on the FEW supply. The goal of this collaborative research is to develop a widely applicable computational protocol, which will be supported by a high-throughput cyberinfrastructure and validated against experimental data, to accelerate the selection of photoactive materials that can efficiently split water (H2O) into hydrogen (H2) and oxygen (O2). At the educational level, this project will promote the emergence of a diverse and well-trained workforce accustomed to collaboration at the frontier of data-driven theory, computation, and experimentation towards solving the outstanding challenges of materials design, which are facing the global FEW system in the twenty-first century.

Technical Abstract: To accelerate the design of new photocatalysts, the research team will exploit novel computational capabilities that extend the scope of conventional quantum-mechanical simulations in describing solar-to-hydrogen conversion. An integrated experimental and computational cycle will be followed to validate the theoretical approach and to assess the effectiveness of advanced performance metrics for the successful selection of new classes of photocatalysts. Specifically, the Schottky barrier height, which sets an upper limit for the solar-to-hydrogen turnover number, will be used as an aggregate of the various performance parameters that collectively contribute to photocatalytic activity. Ultimately, this work will deliver a robust high-throughput framework to guide the optimization of novel photocatalysts with an initial focus on oxynitride and oxysulfide perovskites, taking into account realistic synthetic constraints and conditions of operation. Beyond exploring innovative solutions for solar-to-hydrogen production, the team participants have been and will continue to be actively involved in outreach and undergraduate mentoring in an effort to significantly increase the participation of women and underrepresented minorities in science and engineering and build effective collaborations with international institutions.