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

非技术摘要：从阳光和海水中生产氢燃料有可能深刻重塑食物-能源-水(很少)的格局，并彻底改变用于交通和住宅应用的电力生产。氢是一种可持续的能源载体，它与氧气的催化反应产生电能和热量，而不会排放二氧化碳；该反应唯一的副产品是干净的水。太阳能到氢气的转换提供了不需要农业资源来生产合成燃料的优势，克服了目前对少数供应施加的主要限制之一。这项合作研究的目标是开发一种广泛适用的计算协议，该协议将得到高通量网络基础设施的支持，并根据实验数据进行验证，以加快选择能够有效地将水(H2O)分解为氢(H2)和氧(O2)的光活性材料。在教育层面，这个项目将促进多样化和训练有素的劳动力的出现，他们习惯于在数据驱动的理论、计算和实验的前沿进行合作，以解决材料设计在21世纪面临的突出挑战。技术摘要：为了加快新型光催化剂的设计，研究小组将利用新的计算能力，扩展传统量子力学模拟的范围，描述太阳能到氢的转换。将遵循一个综合的实验和计算周期，以验证理论方法，并评估先进的性能指标对于成功选择新的光催化剂类别的有效性。具体来说，肖特基势垒高度将被用作各种性能参数的集合，这些参数共同有助于光催化活性。肖特基势垒高度设置了太阳能到氢的周转数的上限。最终，这项工作将提供一个强大的高通量框架，以指导新型光催化剂的优化，最初的重点是氮氧化物和硫氧化物钙钛矿，考虑到现实的合成限制和操作条件。除了探索太阳能到氢气生产的创新解决方案外，小组参与者一直并将继续积极参与外联和本科生指导，以努力显著增加妇女和代表不足的少数群体在科学和工程领域的参与，并与国际机构建立有效的合作。

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.