Hydrazone-Based Feedback Loops

基于腙的反馈回路

• 批准号: 2304983
• 负责人: Ivan Aprahamian
• 金额: $ 52.03万
• 依托单位: Dartmouth College
• 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: 2023-07-01 至 2026-06-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2304983&HistoricalAwards=false
• 关键词: Hydrazone; Based; Feedback; Loops

With the support of the Macromolecular, Supramolecular and Nanochemistry Program in the Division of Chemistry, Professor Ivan Aprahamian of Dartmouth College will study how molecular switches can be made to communicate with each other. These studies aim to result in a deeper fundamental understanding of how to control an ensemble of molecules using molecular switches, which in turn will facilitate the understanding of the basic science required to engineer reactions cascades and ensembles, where catalysis, out-of-equilibrium self-assemblies, oscillating systems, among other processes, can be autonomously regulated. The multidisciplinary nature of the project will enable the training and retention of students at different levels of education from high school to undergraduate to graduate students. The group’s public outreach and participation in science, technology, engineering and mathematics (STEM)-related events, such as the annual Science Day at Dartmouth, will help disseminate the group’s work to broader audiences. Moreover, these activities will strengthen and extend the group’s informal and formal science education partnerships and networks with local schools and science museums. In this research, hydrazone-based switches and Zn(II)-initiated negative feedback loops (NFLs) will be used to study how inter-switch communication can be employed for controlling cascade reactions and result in functional products. The straightforward synthesis and modularity of the hydrazone switches and NFL components will allow structure-property analyses for determining the kinetic and thermodynamic factors that control the NFL threshold. With this knowledge at hand, the NFLs will be coupled together in such a way that they can either compete or feed into each other, thus creating interdependency. The NFL will then be used in the synthesis of precise amounts of coordination cages and polymers. Photoreversible ligands will also be developed so light can be used in controlling the concentration of Zn(II) in the solution, while photoacids/bases will be used to tune the solution’s pH. These systems are expected to allow for the clean regulation, using light, of an entire cascade process, thus bringing the approach a step closer to automation.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.

在化学系高分子、超分子和纳米化学项目的支持下，达特茅斯学院的 Ivan Aprahamian 教授将研究如何使分子开关相互通信。这些研究旨在更深入地了解如何进行分子开关。使用分子开关控制分子集合，这反过来将有助于理解设计反应级联和集合所需的基础科学，其中催化、不平衡自组装、振荡系统等过程都可以自主调节，该项目的多学科性质将使从高中到本科生到研究生的不同教育层次的学生能够得到培训和保留。与科学、技术、工程和数学 (STEM) 相关的活动，例如达特茅斯年度科学日，将有助于向更广泛的受众传播该小组的工作，此外，这些活动将加强和扩展该小组的非正式和正式科学。与当地学校和科学博物馆的教育合作伙伴关系和网络在这项研究中，基于腙的开关和锌（II）引发的负反馈回路（NFL）将用于研究如何利用开关间通信来控制级联反应和腙开关和 NFL 组分的直接合成和模块化将允许进行结构特性分析，以确定控制 NFL 阈值的动力学和热力学因素。有了这些知识，NFL 将被耦合。它们可以相互竞争或相互补充，从而产生相互依赖性，然后将用于合成精确数量的配位笼和聚合物，以便将光用于合成。控制溶液中 Zn(II) 的浓度，同时使用光酸/碱的浓度来调节溶液的 pH 值。这些系统预计将能够利用光对整个级联过程进行清洁调节，从而使该方法更加高效。更近一步该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。