EAGER: Controlling active site arrangement in zeolites through OSDA charge distribution

EAGER：通过 OSDA 电荷分布控制沸石中的活性位点排列

• 批准号: 2331027
• 负责人: Daniel Shantz
• 金额: $ 9.14万
• 依托单位: Tulane University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2023
• 资助国家: 美国
• 起止时间: 2023-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2331027&HistoricalAwards=false
• 关键词: EAGER; Controlling; active; site; arrangement

Zeolites are an industrially important class of materials that enable the conversion of low value molecules, for example, the undesirable components of crude oil, into higher value molecules that can be used in transportation fuels and plastics production. Their highly ordered atomic-level structures are what enable these chemical conversions. The ability to control where specific elements are incorporated in these materials would be transformative, leading to improvements in existing technologies, and likely enable new ones such as converting biomass to higher value products. However, this is not currently possible. This EArly-concept Grant for Exploratory Research (EAGER) proposal seeks to change the status quo by developing design criteria to control placement of specific elements in the structure during synthesis. The proposed work is designed such that it will be possible to rapidly assess the transformative potential of the concept, i.e., a low-investment approach with large potential impact. If successful, this will give the scientific community a new approach to controlling the properties of zeolites and other industrially important materials at the atomic level. Zeolites are widely used in catalysis as a result of their discrete pore sizes, controllable framework compositions and exchangeable extra-framework cations. Controlling local structure, most notably the manipulation of the spatial arrangement of framework aluminum, has been a long-sought goal in the research community. The EAGER project seeks to solve this challenge by combining the concepts of using 1) the charge distribution of the organic structure-directing agent (OSDA) and 2) basic insights as to how the OSDA is incorporated in the as-made zeolite to control the arrangement of aluminum i.e., control the active site arrangement. The proposed work plan will enable rapid assessment of the feasibility synthesizing compositionally similar ZSM-12 materials that possess different spatial arrangements of aluminum by using different OSDAs. The ability to modify the spatial arrangement of aluminum in the zeolite framework based on the OSDA charge distribution and knowledge of how the OSDAs pack in the zeolite pores would be transformative, and represent a significant step towards ‘catalysts by design’. Aside from the primary graduate student assigned to the project, an undergraduate student will assist in the project, thus receiving training in zeolite synthesis and characterization methods.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

沸石是工业上重要的一类材料，可以将低价值分子（例如原油中的不良成分）转化为可用于运输燃料和塑料生产的高价值分子，其高度有序的原子级结构。控制这些材料中特定元素的位置的能力将是变革性的，这将导致现有技术的发展，并可能实现新的技术，例如将生物质转化为更高价值的产品。但是，目前这是不可能的。这早期概念探索性研究资助 (EAGER) 提案旨在通过制定设计标准来控制合成过程中特定元素在结构中的放置，从而改变现状。拟议工作的设计使得可以快速评估变革潜力。如果成功，这将为科学界提供一种在原子水平上控制沸石和其他工业重要材料性能的新方法。由于其离散的孔径、可控的骨架组成和可交换的骨架外阳离子，控制局部结构，尤其是骨架铝的空间排列，一直是研究界长期追求的目标。该项目试图通过结合以下概念来解决这一挑战：1）有机结构导向剂（OSDA）的电荷分布和2）关于如何将 OSDA 纳入现有结构的基本见解所提出的工作计划将能够快速评估通过使用不同的 OSDA 来合成具有不同铝空间排列的成分相似的 ZSM-12 材料的可行性。基于 OSDA 电荷分布和 OSDA 如何在沸石孔隙中堆积的知识，铝在沸石框架中的空间排列将是变革性的，代表着向“催化剂”迈出了重要一步。除了分配给该项目的初级研究生外，一名本科生将协助该项目，从而接受沸石合成和表征方法的培训。该奖项反映了 NSF 的法定使命，并通过使用评估被认为值得支持。基金会的智力价值和更广泛的影响审查标准。