DMREF: High-Pressure Synthesis of Novel Oxynitride Photocatalysts Directed by Theory and In Situ Scattering

高压（HP）合成被认为是专业化的和劳动密集型的，具有低通量和成功率。通过将SBU的理论，HP合成和性能测量的安装基础设施与国家同步加速器X射线和中子设施相结合，我们的目标是释放HP作为固态材料发现和开发的常规工具的潜力。晶体结构预测的从头算进化算法提供了可以使用原位散射技术进行实验测试的结构-性能关系。除了精确测定电子和催化性质外，实验结果还提供了一个反馈回路，该回路验证并提高了计算搜索的预测能力。该策略广泛适用于HP探索性合成，并且特别适用于氮氧化物光催化剂的搜索，因为HP有利于固体的产生，而不是导致分解为气体产物的竞争反应。压力还通过仔细控制封闭系统中的O/N的化学计量和排序来促进带隙工程，这是目前在环境压力下使用的氨解途径难以实现的。活性纳米金助催化剂的开发使我们能够快速测试即使是少量回收材料的活性。这笔资金将培养新一代的年轻科学家，他们将适应一种更加综合的方法来开发材料，这种方法将计算和实验高压技术作为主流工具。非物质性虽然高压下的材料合成有可能产生前所未有的变革性材料，但传统的方法是专业化的和劳动密集型的，产量和发现率相对较低。通过将斯托尼布鲁克的理论、合成和性能测量与国家同步加速器X射线和中子设施相结合，我们的目标是释放高压作为固态材料发现的常规工具的潜力。计算搜索将提供目标组合物的列表以及它们的预测性质沿着。 这些目标可以使用高通量技术合成之前，精确测定电子和催化性能。这些结果构成了一个反馈回路，提供了更好的预测能力的洞察力。这种策略特别适用于寻找用于从阳光和水制氢的氮氧化物光催化剂。压力的施加有利于固体的形成，而不是导致分解为气体产物氧气和氮气的竞争反应。活性纳米金助催化剂的最新发展使我们能够快速测试即使是少量回收材料的活性。这笔资金将培养新一代的年轻科学家，他们将采用更综合的材料开发方法，将计算和实验高压技术作为主流工具。

TECHNICALHigh-pressure (HP) synthesis is considered specialized and labor-intensive with low throughput and success rates. By integrating the installed infrastructure for theory, HP synthesis, and property measurements at SBU with national synchrotron x-ray and neutron facilities, we aim to unlock the potential of HP as a routine tool for solid-state materials discovery and development. An ab initio evolutionary algorithm for crystal structure prediction provides structure-property relations that can be tested experimentally using in situ scattering techniques. In addition to the precise determination of electronic and catalytic properties, the experimental results provide a feedback loop that validates and improves the predictive capability of the computational search. This strategy is broadly applicable to HP exploratory synthesis, and particularly suitable in the search for oxynitride photocatalysts, since HP favors production of solids, rather than competing reactions that result in breakdown to gaseous products. Pressure also facilitates band gap engineering through careful control over the stoichiometry and the ordering of O/N in closed systems, something difficult to achieve with current ammonolysis routes used at ambient pressure. The development of active nano-gold co-catalysts allows us to rapidly test the activity of even small amounts of recovered material. The funding will train a new generation of young scientists; comfortable with a more integrated approach to materials development that utilizes computational and experimental high-pressure techniques as mainstream tools.NON TECHNICALAlthough materials synthesis at high pressure has the potential to produce unprecedented and transformative materials, traditional approaches are specialized and labor-intensive, with comparatively low rates of throughput and discovery. By integrating theory, synthesis, and property measurements at Stony Brook with the nation's synchrotron X-ray and neutron facilities, we aim to unlock the potential of high pressure as a routine tool for solid-state materials discovery. Computational search will provide lists of target compositions along with their predicted properties. These targets can be synthesized using high throughput techniques prior to precise determinations of electronic and catalytic properties. These results constitute a feedback loop that provides insight into better predictive capability. This strategy is particularly suitable in the search for oxynitride photocatalysts for use in hydrogen production from sunlight and water. The application of pressure favors the formation of solids rather than competing reactions that result in breakdown to gaseous products, oxygen and nitrogen. The recent development of active nano-gold co-catalysts allows us to rapidly test the activity of even small amounts of recovered material. The funding will train a new generation of young scientists; comfortable with a more integrated approach to materials development that utilizes computational and experimental high-pressure techniques as mainstream tools.