CAREER:Hierarchical Modeling for Rational Catalyst Design in Aqueous Conditions

职业：水相条件下合理催化剂设计的分层建模

• 批准号: 1554385
• 负责人: Rachel Getman
• 金额: $ 50.39万
• 依托单位: Clemson University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-05-01 至 2022-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1554385&HistoricalAwards=false
• 关键词: CAREER; Hierarchical; Modeling; Rational; Catalyst

Abstract (Getman, 1554385)The proposed research will refine molecular simulation models for catalytic reactions in the presence of liquid water and apply the calculations to an electrochemical process for ammonia synthesis that could potentially replace the long-standing, but energy intensive, Haber-Bosch gas phase process. The research is integrated with an educational plan that introduces molecular level simulation concepts to students across levels ranging from high school to graduate research.Theoretical understanding of catalytic materials and processes has advanced significantly in recent years due to rapid improvements in computer resources. This theoretical understanding is streamlining the process of catalyst discovery and moving the field of catalysis toward the prediction of new processes and materials and away from the traditional trial-and-error approach. However, this transition has been slow in the area of liquid phase catalysis, especially electrocatalysis, in large part because of incomplete understanding of the interactions that occur between fluid molecules and the catalyst surface. The research proposed here will take a large step toward better understanding these interactions by considering their free energies, whereas prior treatments have only considered their enthalpies. Traditional modeling equations will be refined and extended by adding, for the first time, free energy contributions due to rotation, translation, and interaction occurring between liquid-phase molecules and species adsorbed to the catalyst surface. The refined models will then be directed toward understanding the reaction between liquid water and gaseous nitrogen in an electrocatalytic environment to produce ammonia under near-ambient temperature and pressure conditions. The improved simulation models will pave the way for a more rational approach to catalyst discovery across a broad range of liquid phase catalytic reactions, and the educational materials will train coming generations of students in molecular-level phenomena and the effective use of molecular simulation tools.

摘要（Getman，1554385）拟议的研究将在存在液态水的情况下完善用于催化反应的分子仿真模型，并将计算应用于氨合成的电化学过程，该过程可能会替代长期的，能量密集的，haber-haber-bosch气体相。 这项研究与一项教育计划融合在一起，该计划向从高中到研究生研究的层次的学生介绍了分子级仿真概念。由于计算机资源的快速改善，对催化材料和过程的理论理解在近年来已大大提高。这种理论上的理解正在简化催化剂发现的过程，并将催化的领域移向新过程和材料的预测，并远离传统的试验方法。 但是，在液相催化，尤其是电催化的区域，这种过渡在很大程度上很大程度上是由于对流体分子与催化剂表面之间发生的相互作用的不完全了解。 这里提出的研究将通过考虑自由能力来更好地理解这些相互作用，而先前的治疗只考虑了它们的焓。 传统的建模方程将通过首次添加由于旋转，翻译和相互作用而引起的液相分子和吸附到催化剂表面的物种之间的自由能贡献来进行完善和扩展。 然后，精制模型将针对理解电催化环境中液态水和气态氮之间的反应，以在近气温和压力条件下产生氨。 改进的仿真模型将为更合理的方法铺平道路，以在广泛的液相催化反应中发现催化剂发现，并且教育材料将培训几代学生的分子级现象和有效使用分子模拟工具。