International Collaboration in Chemistry: CDS&E: Multiscale Simulations of Bifunctional Catalysis

加州大学圣地亚哥分校的 Andreas W Goetz 和特拉华大学的 Dionisios G Vlachos 获得了化学系化学理论、模型和计算方法 (CTMC) 项目以及计算和数据支持的科学与工程 (CDS&E) 项目的奖项支持。 高级网络基础设施部门 (ACI) 共同资助该奖项。 Goetz 和 Vlachos 开发并应用了双功能催化计算工具。该项目是与法国里昂高等师范学院的 Philippe Sautet、Paul Fleurat-Lessard 和 Carine Michel 的国际合作，他们提供了免费的专业知识，并得到了法国 ANR 相应奖项的支持。该项目开发的计算模型和软件能够处理多尺度性质和催化过程固有的复杂性，需要溶液相的双功能催化剂。双功能催化剂对于将生物质转化为液体燃料和化学品非常重要，因此对于不依赖日益减少的石油资源并最大限度地减少全球变暖并产生重大社会影响的可持续未来至关重要。计算机模拟可以在理解这些催化剂如何发挥作用以及指导改进催化剂和工业上可行的工艺的开发方面发挥关键作用。开发的计算方法被集成到免费提供的开源软件库中，并与广泛使用的分子模拟包一起分发。研究生和本科生都参与该项目，高中生和教师也通过实习和研究体验项目来培训下一代科学家。这项工作与化学、化学工程和生物科学等多个领域相关，有助于生物炼制厂的发展，对经济增长和减少二氧化碳排放有明显的推动作用。该项目的进展包括用于快速筛选催化反应网络的新力场和线性能量关系、提取动力学重要步骤的微动力学模拟、使用量子力学/分子力学 (QM/MM) 算法进行分子动力学模拟，允许粒子在 QM/MM 边界上进行自适应交换以确定激活重要反应的能量，以及密度泛函紧束缚理论的参数化，以最大化可访问的时间尺度。这些方法的结合首次能够探索在溶液中使用双功能（金属和酸/碱）催化剂转化生物质的途径的组合爆炸。最初该项目的重点是甘油加氢脱氧成丙二醇，对此有重要的实验数据。这些模拟有助于开发改进的双功能催化剂，最终可以改进生物精炼厂的工艺。作为该项目的一部分，将高效的多尺度模拟方法集成到广泛使用且免费提供的开源软件中可以影响多个应用领域。

Andreas W Goetz of the University of California, San Diego and Dionisios G Vlachos of the University of Delaware are supported by an award from the Chemical Theory, Models and Computational Methods (CTMC) program and the Computational and Data-Enabled Science and Engineering (CDS&E) program in the Chemistry Division. The Division of Advanced Cyberinfrastructure (ACI) is co-funding this award. Goetz and Vlachos develop and apply computational tools for bifunctional catalysis. The project is an international collaboration with Philippe Sautet, Paul Fleurat-Lessard and Carine Michel of the Ecole Normale Superieure de Lyon in France who provide complimentary expertise and who are supported by a corresponding award of the French ANR. This project develops computational models and software capable of handling the multiscale nature and the complexity inherent to the catalytic processes entailing bifunctional catalysts in solution phase. Bifunctional catalysts are important for the conversion of biomass into liquid fuels and chemicals and therefore for a sustainable future that does not rely on dwindling petroleum sources and minimizes global warming with significant societal impact. Computer simulations can play a key role in understanding how these catalysts function and in guiding development of improved catalysts and industrially viable processes. The computational methods developed are integrated into freely available open source software libraries and distributed with a widely used molecular simulation package. Both graduate and undergraduate students are involved in the project, as well as high school students and teachers via internships and research experience programs to train the next generation of scientists. The work has relevance for multiple domains ranging from chemistry to chemical engineering to biosciences and aids the development of biorefineries with a clear impetus on economic growth and reduced CO2 emissions.The developments in this project encompass a new force field and linear energy relations for fast screening of catalytic reaction networks, microkinetic simulations to extract the kinetically important steps, molecular dynamics simulations with quantum mechanics/molecular mechanics (QM/MM) algorithms that allow an adaptive exchange of particles across the QM/MM boundary to determine the activation energies of the important reactions, and parameterizations of density functional tight binding theory to maximize the accessible time scales. The combination of these methods enables for the first time to explore the combinatorial explosion in pathways in the transformation of biomass using bifunctional (a metal and an acid/base) catalysts in solution. Initially the project focuses on the hydrodeoxygenation of glycerol into propanediol, for which significant experimental data is available. These simulations aid in the development of improved bifunctional catalysts that can ultimately lead to improved processes in biorefineries. The integration of efficient multi-scale simulation approaches in widely utilized and freely available open source software as part of this project can impact multiple application domains.