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

DMREF：协作研究：计算和实验相结合，设计用于晶体工程的多功能平台

• 批准号: 1628960
• 负责人: Robert Rioux
• 金额: $ 33.04万
• 依托单位: Pennsylvania State Univ University Park
• 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: 2016-09-01 至 2020-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1628960&HistoricalAwards=false
• 关键词: DMREF; Collaborative; Research; Integration; Computation

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.

1629398/1628960PALMER，JEREMY/RIOUX，ROBERT M.该项目介绍了改进的晶体沸石材料的设计，用于应用，从催化和能源存储到电子设计。 沸石材料的纳米尺寸孔非常适合化学和石油工业中的各种分离和选择性催化转化。提高沸石特性的一个有希望的策略是使用有针对性的合成方法调整晶体形状和尺寸。 该项目的总体目标是开发计算机仿真方法，用于快速识别称为生长修饰符的小分子化合物，可用于控制沸石晶体形状和尺寸。 这将加速新的催化剂，吸附剂和分离材料，以将天然气的廉价和丰富来源转化为燃料和高价值化合物，同时降低有毒排放。 一种在自然和合成结晶中广泛使用的技术来控制晶体习惯和形态，是使用改性剂，它是分子（或大分子）添加剂，它们具有与特定晶体面孔有选择性相关的亲和力，并改变了各向异性的生长速率。 在这一研究领域，无论材料和应用如何，最关键的挑战是对分子水平相互作用和热力学驱动力的不完全理解，这些相互作用和热力学驱动力控制了修饰符对不同晶体表面的吸附和结合特异性。 该项目的重点是整合沸石合成，表征和建模，以开发实验验证的计算平台，以基于平衡吸附属性来表征生长修饰的对结晶的影响。 这将通过解决三个具体目的来实现：（1）使用实验基准数据来预测修饰剂吸附，开发，验证和迭代性完善的密度功能理论和分子模拟模型； （2）评估模型可预测性和转移性到其他修饰材料系统； （3）阐明结构 - 陶艺关系，作为建立修饰符选择准则的一种手段。 这个计算平台将提高我们对管理修饰符功效和特异性的机制的理解，从而为识别有效的修饰符并有可能通过两个数量级来加速其发现，从而为基础提供了基础。 从该项目中获得的基本知识将成为增长修饰符合理设计的转化指南，从而促进了改进的控制结晶过程的策略，以与从催化到分离和吸附和吸附相关的应用。 该项目还将为K-12学生和本科生提供教育和外展成分，包括休斯顿地区高中学生建立分子沸石模型的机会。