CAS: Inhibiting Molecular Reorganization via Strategic Surface Binding

在化学部化学结构、动力学机制-B项目的支持下，佛罗里达州立大学化学和生物化学系的Kenneth Hanson教授试图通过战略性表面结合来理解和控制分子扭曲。分子固有地改变它们的结构（即，这些变形会对它们的性能和效用产生不利影响。 这项研究的目标是使用光学测量来了解表面结合在决定分子性质中的作用，并最终使用这些知识来控制分子的反应性，发射强度和稳定性，以便随后用于更有效的催化，照明，太阳能转换等。作为对这些研究工作的补充，该提案引入了“问科学家游戏”作为一项实时流媒体科学推广奋进。每隔一周，汉森教授都会主持一个不同的博士学位。科学家与社区互动并回答问题。该流是免费的，并提供给所有教育水平，社会经济背景和身份的个人。分子经历结构变化以最小化通过外部刺激（例如压力、氧化剂/还原剂、磁场或光）产生的高能状态的能量。这一过程是所有分子所固有的，但结构的巨大变化，特别是过渡金属配位络合物的结构变化，可能会对其性质和随后在催化、照明、太阳能转换等方面的应用产生破坏性影响。该项目的中心假设是，战略表面结合（即，将多个独立的配体配位到表面）抑制包括刺激的重组，导致激发态寿命、电化学可逆性和高能物质的几何“捕获”增加。为此，本工作的主要目标是1）合成一系列表面结合基序具有系统变化的Cu（I）配位络合物，2）使用光谱和电化学技术来确定表面结合对分子响应刺激的影响，3）几何捕集配位不饱和和反应性Cu（I）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影响审查标准进行评估，被认为值得支持。

With support from the Chemical Structure, Dynamics & Mechanisms-B Program of the Chemistry Division, Professor Kenneth Hanson of the Department of Chemistry and Biochemistry at Florida State University seeks to understand and control molecular distortions by way of strategic surface binding. Molecules inherently change their structure (i.e., distort) in response to external stimuli such as light, heat, magnetic fields, etc. These distortions can have a debilitating impact on their properties and utility. The goal of this research is to use optical measurements to understand the role of surface binding in dictating molecular properties and ultimately use that knowledge to control reactivity, emission intensity, and stability of the molecular for subsequent use in more efficient catalysis, lighting, solar energy conversion, and more. Complementing these research efforts, this proposal introduces "Ask a Scientist Gaming" as a live streaming science outreach endeavor. Every other week, Professor Hanson hosts a different Ph.D. scientist to interface with the community and answer questions. The stream is free and available to individuals of all educational levels, socio-economic backgrounds, and identities. Molecules undergo a structural change to minimize the energy of the high-energy state generated via external stimuli such as pressure, oxidants/reductants, magnetic fields, or light. This process is intrinsic to all molecules but large changes in structure, especially those of transition metal coordination complexes, can have a debilitating impact on their properties and subsequent use in catalysis, lighting, solar energy conversion, and more. The central hypothesis for this project is that strategic surface binding (i.e., coordinating multiple, independent ligands to a surface) inhibits stimuli-included reorganization, resulting in increased excited state lifetimes, electrochemical reversibility, and geometric “trapping” of high energy species. Toward this end, the major goals of this work are to 1) synthesize a series of Cu(I) coordination complexes with systematic variation in the surface binding motif, 2) use spectroscopic and electrochemical techniques to determine the impact of surface binding on the molecules response to a stimulus, 3) geometrically trap coordinatively unsaturated and reactive Cu(I) photolysis products.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.