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

DMREF：理论和原位散射指导的新型氮氧化物光催化剂的高压合成

• 批准号: 1231586
• 负责人: John Parise
• 金额: $ 80万
• 依托单位: SUNY at Stony Brook
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-09-01 至 2017-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1231586&HistoricalAwards=false
• 关键词: DMREF; Pressure; Synthesis; Novel; Oxynitride

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.

高压（HP）合成被认为是专业化和劳动密集型的，产量和成功率低。通过将SBU已安装的理论、HP合成和性能测量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。一种用于晶体结构预测的从头开始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-性质关系。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，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，尤其适用于寻找氮氧化物光催化剂，因为HP倾向于产生固体，而不是导致分解成气态产物的竞争反应。压力还可以通过仔细控制化学计量和封闭系统中O/N的顺序来促进带隙工程，这是目前在环境压力下使用的氨解路线难以实现的。活性纳米金共催化剂的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；熟悉使用计算和实验高压技术作为主流工具的材料开发更综合的方法。尽管高压合成材料具有生产前所未有的变革性材料的潜力，但传统的方法是专业化和劳动密集型的，产量和发现率相对较低。通过将Stony Brook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体材料发现常规工具的潜力。计算搜索将提供目标成分及其预测属性的列表。这些目标可以在精确测定电子和催化性质之前使用高通量技术合成。这些结果构成了一个反馈循环，为更好的预测能力提供了洞察力。这一策略特别适用于寻找用于从阳光和水制氢的氮化氧光催化剂。施加压力有利于固体的形成，而不是导致分解成气态产物、氧和氮的竞争反应。活性纳米金共催化剂的最新发展使我们能够快速测试即使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；熟悉使用计算和实验高压技术作为主流工具的材料开发更综合的方法。