DMREF: Collaborative Research: Integration of Computation and Experiments to Design a Versatile Platform for Crystal Engineering

1629398/1628960 Palmer，Jeremy/Rioux，Robert M.该项目致力于从催化和储能到电子设计等应用中使用的结晶沸石材料的改进设计。 沸石材料的纳米尺寸孔非常适合于化学和石油工业中的各种分离和选择性催化转化。改善沸石性能的一个有前途的策略是使用有针对性的合成方法来调整晶体形状和尺寸。 该项目的总体目标是开发计算机模拟方法，用于快速识别可用于控制沸石晶体形状和尺寸的称为生长改性剂的小分子化合物。 这将加速新型催化剂、吸附剂和分离材料的开发，将廉价而丰富的天然气转化为燃料和高价值化合物，同时降低有毒排放。 在天然和合成结晶中广泛用于控制晶体习性和形态的技术是使用改性剂，改性剂是分子（或大分子）添加剂，其具有选择性吸附在特定晶面上并改变生长的各向异性速率的亲和力。 在这一研究领域中，最关键的挑战，无论材料和应用，是不完整的理解的分子水平的相互作用和热力学驱动力，支配的吸附和结合特异性的改性剂不同的晶体表面。 该项目的重点是整合沸石合成，表征和建模，开发一个实验验证的计算平台，用于表征生长调节剂对结晶的平衡吸附性能的基础上的影响。 这将通过解决三个具体目标来实现：（1）开发，验证和迭代改进密度泛函理论和分子模拟模型，用于使用实验基准数据预测改性剂吸附;（2）评估模型的可预测性和可转移性，以其他改性剂-沸石系统;和（3）阐明结构-性能关系，作为建立改性剂选择指南的一种手段。 这个计算平台将提高我们对调节剂功效和特异性的机制的理解，从而为识别有效的调节剂提供基础，并可能将其发现加速两个数量级。 从这个项目中获得的基础知识将作为一个翻译指导生长调节剂的合理设计，促进发展的改进策略，用于控制结晶过程相关的应用范围从催化分离和吸附。 该项目还将为K-12学生和本科生提供教育和推广组件，包括休斯顿地区高中生建立分子沸石模型的机会。

1629398/1628960Palmer, Jeremy/Rioux, Robert M.The project addresses improved designs of crystalline zeolite materials used in applications ranging from catalysis and energy storage to electronics design. The nanometer sized pores of the zeolite materials are ideally suited for a wide range of separations and selective catalytic conversions in the chemical and petroleum industries. A promising strategy for improving the properties of zeolites is to tune crystal shape and size using targeted synthetic approaches. The overall goal of this project is to develop computer simulation methods for rapidly identifying small-molecule compounds known as growth modifiers that can be used to control zeolite crystal shape and size. This will accelerate the development of new catalysts, adsorbents, and separations materials for converting inexpensive and abundant sources of natural gas into fuels and high-valued compounds while simultaneously lowering toxic emissions. A technique that is broadly utilized in both natural and synthetic crystallization to control crystal habit and morphology is the use of modifiers, which are molecular (or macromolecular) additives that possess an affinity for selectively adsorbing on specific crystal faces and altering the anisotropic rate(s) of growth. The most critical challenge in this field of research, irrespective of the material and application, is the incomplete understanding of the molecular-level interactions and thermodynamic driving forces that govern the adsorption and binding specificity of modifiers to different crystal surfaces. The focus of this project is to integrate zeolite synthesis, characterization, and modeling to develop an experimentally-validated computational platform for characterizing growth modifier effects on crystallization based on equilibrium adsorption properties. This will be achieved by addressing three specific aims: (1) develop, validate, and iteratively refine density functional theory and molecular simulation models for predicting modifier adsorption using experimental benchmark data; (2) assess model predictability and transferability to other modifier-zeolite systems; and (3) elucidate structure-property relationships as a means of establishing guidelines for modifier selection. This computational platform will improve our understanding of the mechanisms governing modifier efficacy and specificity, thereby providing a foundation for identifying effective modifiers and potentially accelerating their discovery by two orders of magnitude. The fundamental knowledge gained from this project will serve as a translational guide for the rational design of growth modifiers, fostering the development of improved strategies for controlling crystallization processes relevant to applications ranging from catalysis to separations and adsorption. The project will also provide educational and outreach components to K-12 students and undergraduates, including opportunities for Houston-area high school students to build molecular zeolite models.