NSF/DOE Solar Hydrogen Fuel: Accelerated Discovery of Advanced RedOx Materials for Solar Thermal Water Splitting to Produce Renewable Hydrogen

首席调查者：Charles B.MusgraveNumber：1433521非技术描述为满足全球能源和化学需求，开发化石燃料的可再生替代品日益迫切。氢气是一种很有前途的可再生燃料，可以从可持续资源中制取。生产可再生氢燃料的一种特别有希望的方法是太阳能热水分解(STWS)，即在高温下，在催化剂材料的存在下，利用太阳能的热量将水分解为氢燃料和氧气。为了高效地利用STWS生产氢气，必须应对两个技术挑战。第一个挑战是发现能够有效驱动热水分解的催化剂材料，第二个挑战是开发一种反应系统来收集太阳能并高效地将其输送到水分解反应中。在这方面，一个主要问题是，典型的STWS过程的温度变化高达500摄氏度，这对催化剂材料的稳定性和催化剂材料所在的反应过程造成了严重的压力。最近，首席研究员S团队开发了一种恒温运行的太阳能热水分解过程。该项目的目标是发现利用这一恒温过程的新的STWS材料。新的STWS材料将通过加速筛选过程被发现，该过程包括材料的计算原型和对这些预测的实验验证。研究人员可通过公开的网上数据库评估材料筛选研究的相关数据。该项目活动将培训两名研究生和一批本科生，掌握材料筛选的先进技术，这可能对材料行业有价值。这项研究还将被纳入科罗拉多大学博尔德分校的工程、材料科学和化学课程。技术描述生产可再生氢燃料的一个有前途的方法是太阳能热水分解(STWS)，在高温下，太阳能的热输入被用来在氧化还原材料存在的情况下将水分解为氢燃料和氧气，在高温下，反应热力学和动力学是有利的。典型的STWS工艺的温度波动高达500摄氏度，这给催化剂材料和催化剂材料所在的反应器的稳定性带来了严重的压力。最近，首席研究员S团队开发了一种恒温运行的太阳能热水分解过程。该项目的目标是发现新的等温STWS氧化还原活性材料，利用这一恒温过程。该方法包括使用提高精度的从头计算量子模拟进行多阶段筛选，以向下选择性能最佳的候选氧化还原材料，然后进行实验验证和模型改进。快速筛选工具还将评估用于太阳热化学反应堆模型的限速表面反应的动力学。这种加速的材料发现方法将扩展到筛选用于等温水分解的多组分金属氧化物氧化还原活性物质。该项目还包括提供更广泛影响的活动。两名研究生和一些本科生将接受高级材料筛选工具和相关计算方法的培训，这些工具和相关的计算方法可能对未来的材料行业很重要。由于筛选工作将产生大量材料数据，这些数据可能对研究金属氧化物的研究人员有用，因此将创建一个可公开访问的在线数据库，其中包含计算出的形成热和带隙。将为科罗拉多大学博尔德分校开发用于材料筛选的课程模块。

Principal Investigator: Charles B. MusgraveNumber: 1433521Nontechnical Description There is growing urgency to develop renewable alternatives to fossil fuels for satisfying global energy and chemical demands. Hydrogen gas is a promising renewable fuel which can be made from sustainable resources. One particularly promising route to produce renewable hydrogen fuels is solar thermal water splitting (STWS), in which the heat of solar energy is used to split water into hydrogen fuel and oxygen in the presence of a catalyst material at high temperatures. To efficiently produce hydrogen gas by STWS, two technical challenges must be met. The first challenge is the discovery of catalyst materials that can efficiently drive thermal water splitting, and the second challenge is to develop a reaction system to collect solar energy and deliver it efficiently to the water splitting reaction. In this regard, a major problem is that typical STWS processes have temperature changes of up to 500 degrees Celsius, which puts severe stress of the stability of the catalyst materials and the reaction process that the catalyst material is contained in. Recently, the principal investigator?s team has developed a solar thermal water splitting process that operates at constant temperature. The goal of this project is to discover new STWS materials which exploit this constant temperature process. New STWS materials will be discovered through an accelerated screening process which involves computational prototyping of materials and experimental validation of these predictions. Relevant data from the materials screening studies will be assessable to researchers through a publically available web-based database. The project activities will train two graduate students and number of undergraduate students in advanced techniques for materials screening which may valuable for the materials industry. The research will also be incorporated into engineering, materials science and chemistry courses at the University of Colorado, Boulder.Technical Description A promising route to produce renewable hydrogen fuels is solar thermal water splitting (STWS), in which the thermal input from solar energy is used to drive the splitting of water into hydrogen fuel and oxygen gas in the presence of a RedOx material at high temperatures where the reaction thermodynamics and kinetics are favorable. Typical STWS processes have temperature swings of up to 500 degrees Celsius, which puts severe stress of the stability of the catalyst materials and the reactor that the catalyst material is contained in. Recently, the principal investigator?s team has developed a solar thermal water splitting process that operates at constant temperature. The goal of this project is to discover new isothermal STWS RedOx active materials which exploit this constant temperature process. The approach involves multistage screening using ab initio quantum simulations of increasing accuracy to down-select candidate RedOx materials with the best performance, followed by experimental validation and refinement of the model. Rapid screening tools will also assess the kinetics of rate-limiting surface reactions for use in solar thermal chemical reactor models. This accelerated materials discovery approach will be expanded to screen for multicomponent metal oxide RedOx active materials for isothermal water splitting. The project also includes activities to provide broader impacts. Two graduate students and a number of undergraduate students will gain training in advanced material screening tools and associated computational methodology which are likely to be important for the materials industries in the future. Since the screening efforts will generate vast quantities of materials data which may be useful to researchers studying metal oxides, a publicly accessible online database will be created containing the calculated heats of formation and band gaps. Course modules for materials screening will be developed for University of Colorado, Boulder.