Quantitative assessment of non-covalent interactions in aqueous medium and in hydrophobic cavities using Cucurbiturils

使用葫芦脲定量评估水介质和疏水腔中的非共价相互作用

• 批准号: 1905238
• 负责人: Eric Masson
• 金额: $ 45.5万
• 依托单位: Ohio University
• 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: 2019-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1905238&HistoricalAwards=false
• 关键词: Quantitative; assessment; non; covalent; interactions

Living organisms, from single cells to human beings, thrive as a result of an extremely large number of interactions and reactions between molecules that include proteins, DNA, sugars and lipids. Drugs also interact with these chemical structures to counteract symptoms and diseases. A more precise knowledge of how different chemical structures interact (or "stick" together) has the potential to enable a better understanding of biochemical processes involved in diseases and to facilitate drug design. With the support of the NSF Macromolecular, Supramolecular and Nanochemistry (MSN) Program, the research group of Professor Eric Masson at Ohio University designs and synthesizes hollow, pumpkin-shaped molecules that can accommodate two chemical entities in its hollow center. By bringing two chemical entities together, the Masson group seeks to determine how well they interact and to quantify the strength of their interactions at the molecular level. The research project involves graduate and undergraduate students (including students from underprivileged backgrounds) and trains them in organic, analytical and computational chemistry. Among other outreach activities, Professor Masson also co-organizes a yearly science communication and policy workshop held at Ohio University and at the University of Leipzig, Germany. The workshop brings together students from chemistry, journalism and international studies at both institutions around scientific themes of societal interest. Through the workshop, students learn to communicate scientific concepts to non-scientists.For the purpose of quantifying non-covalent interactions in both aqueous medium and in hydrophobic cavities surrounded by an aqueous environment, Professor Masson's group designs supramolecular systems that are water-compatible, versatile for evaluating a wide range of non-covalent interactions; and geometrically well-defined and far less complex than natural systems, to avoid secondary perturbations. There are three specific aims in this project. In the first aim, the Cucurbituril (CB[n]) family of macrocycles is used to encapsulate highly hydrophilic guests and determine the strengths of the intramolecular hydrogen bonds formed inside the hydrophobic cavity of CB[n]. In the second aim, "2:1 stacked" ternary complexes of a variety of 4'- substituted platinum(II) terpyridyl complexes in curcubit[8]urils (CB[8]) are designed. These ternary complexes serve as self-sorting probes for quantifying Coulombic interactions between peptides as well as aryl-aryl "pi-pi" and aryl-cycloalkenyl CH-pi interactions in aqueous medium. The last aim exploits the use of the "2:1 stacked" ternary complexes as supramolecular balances for quantifying dispersive "pi-pi" and CH-pi interactions in aqueous medium. The supramolecular balance is formed by self-sorting of a platinum complex connected to a triptycene unit (the "wheel") with another platinum complex without triptycene (the "shaft") in CB[8]. The novel ternary complexes that are composed of one "shaft" and one "wheel" in CB[8] or two "wheels" in CB[8] may represent new families of supramolecular brakes and spur gears.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.

从单个细胞到人类的生物体由于包括蛋白质，DNA，糖和脂质的分子之间的相互作用和反应而壮成长。药物还与这些化学结构相互作用以抵消症状和疾病。更精确的了解不同的化学结构如何相互作用（或“粘在一起”）有可能更好地了解涉及疾病涉及的生化过程并促进药物设计。在NSF大分子，超分子和纳米化学（MSN）计划的支持下，俄亥俄州大学设计的Eric Masson教授研究小组合成了空心的南瓜形分子，可以容纳其空心中心的两个化学实体。通过将两个化学实体聚集在一起，Masson群体试图确定它们相互作用的效果，并在分子水平上量化其相互作用的强度。该研究项目涉及研究生和本科生（包括来自贫困背景的学生），并培训他们进行有机，分析和计算化学。除其他外展活动外，马森教授还共同组织了在俄亥俄州大学和德国莱比锡大学举行的年度科学传播和政策研讨会。 该研讨会汇集了两个机构的化学，新闻和国际研究的学生，围绕社会利益的科学主题。通过研讨会，学生学会将科学概念传达给非科学家。为了量化水性培养基和疏水腔中的非共价相互作用，被水性环境包围，Masson教授的群体设计超分子系统具有水，可用于评估非可比价互动的广泛范围的水。并且几何定义明确且比天然系统要复杂得多，以避免次要扰动。 该项目有三个具体的目标。在第一个目标中，大环的葫芦（CB [n]）家族用于封装高度亲水的客人，并确定CB疏水腔内形成的分子内氢键的强度[N]。 在第二个目标中，设计了curcubit [8]尿液（CB [8]）中各种4'-取代铂（II）terpyridyl络合物的“ 2：1”的三元复合物。这些三元络合物用作自我分级探针，用于量化肽以及芳基 - 芳基芳基的“ PI-PI”和芳基 - cycloalkenyl CH-PI相互作用之间的库仑相互作用。最后的目标利用了“ 2：1堆叠”三元络合物作为量化色散“ PI-PI”和CH-PI相互作用的超分子平衡的使用。超分子平衡是通过将CB [8]中的另一个没有三倍苯酮（“轴”）的铂型复合物（“轴”（“轴”）相连的铂络合物（“车轮”）相连的铂综合体（“车轮”）。 The novel ternary complexes that are composed of one "shaft" and one "wheel" in CB[8] or two "wheels" in CB[8] may represent new families of supramolecular brakes and spur gears.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.

项目成果

Light- and Chemical-Doping-Induced Magnetic Behavior of Eu Molecular Systems

• DOI: 10.1021/acs.inorgchem.3c01154
• 发表时间: 2023-07-28
• 期刊: INORGANIC CHEMISTRY
• 影响因子: 4.6
• 作者: Rajh，Tijana;Masson，Eric;Hla，Saw-Wai
• 通讯作者: Hla，Saw-Wai