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

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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.