Exploring the contributions of multiple physical forces towards the self-assembly of complex macroions in solution

探索多种物理力对溶液中复杂大离子自组装的贡献

• 批准号: 1904397
• 负责人: Tianbo Liu
• 金额: $ 46万
• 依托单位: University of Akron
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-10-01 至 2023-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1904397&HistoricalAwards=false
• 关键词: Exploring; contributions; multiple; physical; forces

Many biological molecules, such as proteins and DNA, contain many charged (ionic) groups of the same kind. A phenomenon observed in these molecules is that they can associate with each other in water despite the fact that positively-charge groups repel other positively-charged groups (or negative charges repel negative charges). Professor Tianbo Liu of the University of Akron designs and studies complex charged molecules that are large and water-soluble, and that attract each other even when they carry the same charge (positive or negative). Through an investigation of how different kinds of inter-molecular forces cooperate and compete with each other in solution, the Liu group gains a better understanding of how such ions attract one another. The conclusions are expected to be applicable to many other solution systems, and instructive for understanding biological solutions. The project contributes fundamentally to many science disciplines including physical chemistry, supramolecular chemistry, biochemistry, and materials sciences. In addition, the ability to manipulate the strengths and the effects of different inter-molecular forces would enable the design of novel self-assembled structures for applications in nanotechnology or biotechnology. This project provides research training to high school, undergraduate and graduate students, preparing them for further education or careers in STEM fields.Between simple ionic solutions (e.g., sodium chloride) and the suspensions of bulky colloidal particles, there exists a region of macroions - nanoscaled soluble ions. Supported by the Macromolecular, Supramolecular and Nanochemistry Program, Professor Liu expands his research project from the study of purely hydrophilic macroions, dominated by electrostatic interactions in polar solvents, to more complicated macroions with other forces (hydrophobic, cation-pi, pi-pi, etc.) also being present. The cooperation and competition of various intermolecular forces in such macroionic solutions are expected to demonstrate rich assembly phenomena. There are three main objectives in this project. First, the project aims to understand the effect of functionalization of macroions with organic groups on the properties of such ions in polar solvents. Secondly, dumbbell-shaped macroions with polymerizable hydrophobic linkers are designed, synthesized, then assembled into single-layered hollow, spherical "blackberry-like" structures. Polymerization of the linkers is expected to create stable, porous nanocontainers. Finally, the effects of aromatic groups on the counterion distribution around the macroions and how it leads to various controllable assembly structures are examined.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.

许多生物分子，如蛋白质和DNA，含有许多相同种类的带电（离子）基团。 在这些分子中观察到的现象是，尽管带正电荷的基团排斥其他带正电荷的基团（或负电荷排斥负电荷），但它们可以在水中彼此缔合。 阿克伦大学的Tianbo Liu教授设计和研究了复杂的带电分子，这些分子很大，而且是水溶性的，即使它们携带相同的电荷（正电荷或负电荷），也会相互吸引。 通过研究不同种类的分子间力如何在溶液中相互合作和竞争，Liu小组更好地理解了这些离子如何相互吸引。 所得结论对其他溶液体系具有一定的指导意义，对理解生物溶液具有一定的指导意义。 该项目为许多科学学科做出了根本性的贡献，包括物理化学，超分子化学，生物化学和材料科学。 此外，操纵不同分子间力的强度和效果的能力将使设计用于纳米技术或生物技术的新型自组装结构成为可能。 该项目为高中生、本科生和研究生提供研究培训，为他们在STEM领域的进一步教育或职业生涯做好准备。氯化钠）和大体积胶体颗粒的悬浮液中，存在大离子-纳米级可溶性离子区域。 在大分子、超分子和纳米化学项目的支持下，刘教授将他的研究项目从极性溶剂中以静电相互作用为主的纯亲水性大离子的研究扩展到具有其他力（疏水性、阳离子-pi、pi-pi等）的更复杂的大离子。也在场。 在这种大离子溶液中，各种分子间力的合作和竞争有望表现出丰富的组装现象。 该项目有三个主要目标。 首先，该项目旨在了解有机基团对大离子功能化对极性溶剂中此类离子性质的影响。 其次，设计、合成了具有可聚合疏水连接基的哑铃形大离子，并将其组装成单层中空球形的“黑莓状”结构。 预期连接体的聚合产生稳定的多孔纳米容器。 最后，研究了芳香族基团对大离子周围反离子分布的影响，以及它如何导致各种可控组装结构。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的评估被认为值得支持影响审查标准。

项目成果

Supramolecular structures based on metal-organic cages

• DOI: 10.1016/j.giant.2021.100050
• 发表时间: 2021-03
• 期刊: IEEE Transactions on Medical Imaging
• 影响因子: 10.6
• 作者: Ehsan Raee;Yuqing Yang;Tianbo Liu

Abnormal Association between Metal−Organic Cages and Counterions Regulated by the Hydration Shells

金属有机笼与水合壳调节的反离子之间的异常关联

• DOI: 10.1002/chem.202104332
• 发表时间: 2022
• 期刊: Chemistry – A European Journal
• 作者: Yang, Yuqing;Raee, Ehsan;Liu, Tianbo
• 通讯作者: Liu, Tianbo

Oligo( l -glutamic acids) in Calcium Phosphate Precipitation: Mechanism of Delayed Phase Transformation

磷酸钙沉淀中的低聚（L-谷氨酸）：延迟相变机制

• DOI: 10.1021/acs.jpcb.0c01690
• 发表时间: 2020
• 期刊: The Journal of Physical Chemistry B
• 作者: Ustriyana, Putu;Michel, F. Marc;Wilson, Michael C.;Harmon, Emma;Chen, Jiahui;Liu, Tianbo;Sahai, Nita
• 通讯作者: Sahai, Nita

Accurate Determination of the Quantity and Spatial Distribution of Counterions around a Spherical Macroion

准确测定球形宏离子周围反离子的数量和空间分布

• DOI: 10.1002/ange.202013806
• 发表时间: 2021
• 期刊: Angewandte Chemie
• 作者: Chen, Jiahui;Bera, Mrinal K.;Li, Hui;Yang, Yuqing;Sun, Xinyu;Luo, Jiancheng;Baughman, Jessi;Liu, Cheng;Yao, Xuesi;Chuang, Steven S. C.
• 通讯作者: Chuang, Steven S. C.

Co-ion Effects in the Self-Assembly of Macroions: From Co-ions to Co-macroions and to the Unique Feature of Self-Recognition

• DOI: 10.1021/acs.langmuir.0c01797
• 发表时间: 2020-09-08
• 期刊: LANGMUIR
• 影响因子: 3.9
• 作者: Chen, Jiahui;Qian, Kun;Liu, Tianbo
• 通讯作者: Liu, Tianbo