CAREER: Computational Studies of Aromaticity-Modulated Interactions in Supramolecular Chemistry

职业：超分子化学中芳香性调节相互作用的计算研究

• 批准号: 1751370
• 负责人: Judy I-Chia Wu
• 金额: $ 58.43万
• 依托单位: University of Houston
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-03-01 至 2023-02-28
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1751370&HistoricalAwards=false
• 关键词: CAREER; Computational; Studies; Aromaticity; Modulated

Hydrogen bonds are weak chemical interactions that, like the "glue" used to stick items together, can hold many molecules together to create elaborate chemical structures or to perform sophisticated functions. These interactions underlie many biological processes (e.g., DNA replication and enzyme catalysis) which, when artfully mimicked in man-made materials, can have important applications for biomedical, environmental, and renewable energy fields. However, factors that influence the strengths of hydrogen bonds (i.e., how "sticky" they are) in these complex systems remain largely convoluted, making "copying nature" in man-made materials difficult. In this project, Prof. Judy Wu and her students at the University of Houston are applying computational tools to study how hydrogen bonds work in concert in large complex organic molecules. Her research aims to establish new and useful ways of controlling hydrogen bonds, and to demonstrate their broader impacts for the discovery of advanced materials (e.g., gels, plastics, and electronics with novel properties). Integrated to this project are plans to develop a "Numbers to Insights" student workshop and web application to help facilitate the exchange of scientific ideas and findings across computational and experimental chemistry research groups. The proposed project aims to show that the marriage of two fundamental chemical concepts, aromaticity and hydrogen bonding, gives rise to surprising reciprocal effects with important consequences for supramolecular chemistry. Despite the recognition of hydrogen bonding and aromaticity as largely separate concepts in organic chemistry, research from the Wu group is showing that aromaticity can be used to control the strengths of intermolecular hydrogen bonding interactions through a phenomena called aromaticity-modulated hydrogen bonding (AMHB). Computational quantum chemical tools are applied to test the AMHB relationship at the 1) ground and 2) excited states of hydrogen-bonded molecular recognition units, 3) to investigate how AMHB influences the self-assembly modes of hydrogen-bonded molecular building blocks, and 4) to elucidate the role of AMHB in some examples of enzyme catalysis. At the core of this CAREER project is the vision to bridge discoveries of novel chemical relationships to their probable impacts in supramolecular chemistry.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.

氢键是弱化学相互作用，就像用来将物品粘在一起的“胶”一样，可以将许多分子固定在一起以创建精美的化学结构或执行复杂的功能。这些相互作用是许多生物学过程（例如，DNA复制和酶催化）的基础，当在人造材料中巧妙地模仿它，可以在生物医学，环境和可再生能源领域中使用重要的应用。但是，影响这些复杂系统中氢键强度（即它们的“粘性”）的强度仍然很大程度上令人费解，从而使人造材料中的“复制性质”变得困难。在这个项目中，休斯顿大学的朱迪教授和她的学生正在应用计算工具来研究氢键如何在大型复杂有机分子中共同起作用。她的研究旨在建立控制氢键的新的和有用的方法，并证明它们对发现高级材料的更广泛影响（例如凝胶，塑料和具有新颖性能的电子产品）。与该项目集成在一起的计划是开发“数字来见解”学生研讨会和Web应用程序，以帮助促进在计算和实验化学研究小组之间交流科学思想和发现。 拟议的项目旨在表明，两个基本化学概念（芳香族性和氢键）的结合产生了令人惊讶的倒数效应，对超分子化学产生了重要影响。尽管氢键和芳香性在很大程度上是有机化学中的概念，但WU组的研究表明，芳香族性可用于控制分子间氢键相互作用的强度，这是通过称为芳族性调节的氢键（AMHB）的现象（AMHB）。计算量子化学工具用于在1）地面和2）氢键分子识别单元的激发状态下测试AMHB关系，3）研究AMHB如何影响AMHB的自组成模式，以阐明AMHB在某些Enzyme catalsy catalsysissy emhb中的作用。这个职业项目的核心是构成新的化学关系发现的愿景，使其可能在超分子化学中产生影响。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子和更广泛影响的评估审查标准来通过评估来获得支持的。

项目成果

How does excited-state antiaromaticity affect the acidity strengths of photoacids?

激发态反芳香性如何影响光酸的酸性强度？

• DOI: 10.1039/d0cc02952a
• 发表时间: 2020
• 期刊: Chemical Communications
• 影响因子: 4.9
• 作者: Wen, Zhili;Karas, Lucas José;Wu, Chia-Hua;Wu, Judy I-Chia
• 通讯作者: Wu, Judy I-Chia

Self-assembling purine and pteridine quartets: how do π-conjugation patterns affect resonance-assisted hydrogen bonding?

自组装嘌呤和蝶啶四重体：α-共轭模式如何影响共振辅助氢键？

• DOI: 10.1039/c9ob02412c
• 发表时间: 2020
• 期刊: Organic & Biomolecular Chemistry
• 影响因子: 3.2
• 作者: Paudel, Hari Ram;Das, Ranjita;Wu, Chia-Hua;Wu, Judy I.
• 通讯作者: Wu, Judy I.

Hydrogen bond design principles

• DOI: 10.1002/wcms.1477
• 发表时间: 2020-05-16
• 期刊: WILEY INTERDISCIPLINARY REVIEWS-COMPUTATIONAL MOLECULAR SCIENCE
• 影响因子: 11.4
• 作者: Karas, Lucas J.;Wu, Chia-Hua;Wu, Judy I-Chia
• 通讯作者: Wu, Judy I-Chia

Baird’s rules at the tipping point

• DOI: 10.1038/s41557-022-00988-z
• 发表时间: 2022-07
• 期刊: Nature Chemistry
• 影响因子: 21.8
• 作者: L. Karas;J. Wu

Aromaticity gain increases the inherent association strengths of multipoint hydrogen-bonded arrays

芳香度增益增加了多点氢键阵列的固有缔合强度

• DOI: 10.1039/c8cc00422f
• 发表时间: 2018
• 期刊: Chemical Communications
• 影响因子: 4.9
• 作者: Wu, Chia-Hua;Zhang, Yu;van Rickley, Krista;Wu, Judy I.
• 通讯作者: Wu, Judy I.