Enabling high-throughput computational discovery of stable and active single-site oxidation catalysts

该项目将推进计算工具，用于发现，设计和机械理解促进含有单一，高度特异性活性位点的催化剂反应的因素。 这种单位点催化剂为改善一系列催化反应的活性和产物选择性提供了独特的机会。 计算工具的开发将侧重于构成天然气主要成分的轻质烷烃的脱氢。 丰富的页岩气资源已经带来了对更有效的催化剂的日益增长的需求，所述催化剂用于将相对不活泼的烷烃转化为更活泼的物种，所述更活泼的物种作为制造多种化学品和燃料的中间体而具有价值。 新的计算工具的开发将加速有效的单活性中心催化剂的鉴定，从而为化学和石油工业提供保持我国在化学和能源经济部门的竞争力所需的新催化剂。 单活性中心催化剂为高选择性和高活性提供了独特的机会，但其研究和设计仍然存在挑战。 计算催化已经成为一个强大的工具-当与实验研究相结合时-指导基于基本结构-活性关系的催化剂设计，而不是通常使用的低效试错方法。 该项目将推进计算工具的发现，设计和单中心催化剂的机理研究。 计算平台将结合联合收割机的催化剂结构的建设和发展的新方法，提高第一原理预测精度的方法。 新的迭代筛选方法将赋予基本的理解，结构-性质的关系，产生气相氧化剂活化的选择性C-H活化具有高稳定性。 研究工作将集中在三个目标上：1）建立高通量的单位点催化剂结构生成工具; 2）开发强大的增强DFT（密度泛函理论）预测能量学; 3）生成迭代设计策略，用于发现稳定和活性的单位点催化剂。 这三个目标将带来一个强大的开源平台，用于发现利用页岩资源中丰富的能源和化学原料储备所需的催化剂。 从更广泛的角度来看，开源软件工具和结构-性质相关性将为计算催化社区提供超越本工作中研究的单中心催化剂的益处。 该项目将研究生和本科生的教育与计算催化剂设计的创新研究相结合。 这项研究将通过在马萨诸塞州理工学院博物馆为波士顿地区学校的6-12年级学生举办的实践研讨会与社区分享，特别强调让女性和代表性不足的少数民族参与STEM。 当地的努力将通过向普通观众教授化学、催化和电子结构的在线教程得到加强。

The project will advance computational tools for the discovery, design, and mechanistic understanding of factors promoting reactions on catalysts containing a single, highly-specific active site. Such single-site catalysts offer unique opportunities for improving the activity and product selectivity of a range of catalytic reactions. The computational tool development will focus on the dehydrogenation of light alkanes that comprise the major component of natural gas. The abundance of shale gas resources has brought increasing need for more efficient catalysts for transforming the relatively unreactive alkanes to more reactive species of value as intermediates in the manufacture of a wide range of chemicals and fuels. Development of the new computational tools will hasten the identification of efficient single-site catalysts, thus providing the chemical and petroleum industries with new catalysts needed to maintain our Nation's competitiveness in the chemicals and energy sectors of the economy. Single-site catalysts present unique opportunities for high-selectivity and activity, but challenges remain for their study and design. Computational catalysis has emerged as a powerful tool - when coupled with experimental studies - to guide the design of catalysts based on fundamental structure-activity relationships rather than the inefficient trial-and-error approach often used. The project will advance computational tools for discovery, design, and mechanistic study of single-site catalysts. The computational platform will combine new methodology for catalyst structure building and development, with methods for improving first-principles prediction accuracy. New iterative screening approaches will impart fundamental understanding to structure-property relationships that give rise to gas phase oxidant activation for selective C-H activation with high stability. The research efforts will focus on three aims: 1) building high-throughput single-site catalyst structure generation tools; 2) developing robust augmented-DFT (density functional theory) predictions for energetics; and 3) generating iterative design strategies for discovering stable and active single-site catalysts. These three aims will bring to bear a robust, open-source platform for the discovery of catalysts needed to capitalize on the abundant energy and chemical feedstock reserves found in shale resources. From a broader perspective, the open-source software tools and structure-property correlations will provide benefit to the computational catalysis community beyond the single-site catalysts studied in this work. The project integrates the education of graduate and undergraduate students with innovative research in computational catalyst design. The research will be shared with the community through a hands-on workshop at the Massachusetts Institute of Technology Museum for grades 6-12 students in Boston-area schools, with a special emphasis on engaging female and underrepresented minorities in STEM. Local efforts will be augmented by online tutorials that teach chemistry, catalysis, and electronic structure to a general audience.