Coordination Chemistry Using Strategic Design of Ligands: Fundamental Explorations and Applications

在这项研究计划中，我们将解决以下问题：我们如何为改进分子设计做出贡献：(1)感知环境（氧-）阴离子，(2)产生磁性分子？(3)我们如何“开启”和“关闭”分子磁性？我们将解决这些问题，因为：(1)虽然氧阴离子对多个生命周期至关重要，但像磷酸盐一样，氧阴离子也会导致水生生态系统的富营养化（即植物物质的过度生长和动物因缺氧而死亡），因此可以用于感知磷酸盐的材料是理想的。我们之前已经证明了我们的分子能够吸引氧阴离子。了解新的结构功能关系将有助于进一步开发更好的传感器，这对于日益严格的法规所要求的较低检测限至关重要。该研究将产生一个受体库，用于筛选广泛的阴离子分析物，这对全球需要环境修复的地区至关重要。(2)自从1993年第一次报道分子磁体以来，人们对这类分子有着极大的热情，因为它们可以用作磁性存储设备和量子比特（换句话说，它们可以用于量子计算）。其中一个仍然存在的挑战是让这些分子在室温下表现得像磁铁一样（因为许多分子只在绝对零度附近起作用！）在提议的研究中，我们正在制造可调谐的有机分子来与金属阳离子相互作用，这将使我们能够调整新的分子磁体的功能。通过改变与自旋活性金属相互作用的有机成分，我们将有助于改进独特的和未开发的分子磁性材料的分子设计。实现磁性器件应用的一个步骤是在分子磁铁中加入一个“开关”。在提议的研究中，我们将在我们的有机成分中引入功能来“打开”和“关闭”分子磁性。我们建议通过三种方式做到这一点：通过(a)加入氧化还原活性位点；或(b)构建氧化还原活性有机骨架；(3)利用光来改变分子的构象。这些方法将使我们能够在分子水平上为我们的系统诱导一个开关。我们提出的研究所产生的知识将被我们和其他人用于推进环境阴离子检测和分子磁学领域。我们的研究小组在单晶x射线结构和磁性分析方面具有独特的专业知识，结合起来，我们将在结构-功能关系方面提供新的见解。这种环境将为学员提供极好的发展技能的机会，使他们能够为学术、政府和工业研究实验室做出贡献，确保该研究项目将造福于更大的加拿大社区。

In this research proposal, we will address the questions: How can we contribute to improved molecular design for (1) sensing environmental (oxo-)anions, and (2) producing magnetic molecules? (3) How can we `turn on' and `turn off' molecular magnetic properties? We will address these questions because: (1) While essential to multiple life cycles, oxo-anions, like phosphate, can also cause eutrophication of aquatic ecosystems (that is, the overgrowth of plant matter, and death of animals due to lack of oxygen), and therefore materials that can be used for sensing of phosphate are desirable. We have previously demonstrated that our molecules are able to attract oxo-anions. Understanding of new structure-function relationships will enable further development of better sensors which is essential for lower detection limits required by increasingly stringent regulations. The proposed research will generate a library of receptors for screening a wide array of anionic analytes, which is critical in global regions in need of environmental remediation. (2) Since the first reported molecular magnets in 1993, there has been great enthusiasm for this class of molecules because they could have use as magnetic storage devices and for use as qubits (in other words, they could be used in quantum computing). One of the challenges that still exists is getting these molecules to behave like magnets at room temperature (since many function only near absolute zero!) In the proposed research, we are making tunable organic molecules to interact with metal cations, which will enable us to adjust the functionality of new molecular magnets. By varying organic components which interact with spin active metals, we will contribute to the improved molecular design of unique and untapped molecular magnetic materials. (3) One step towards achieving magnetic device applications is the incorporation of a "switch" into the molecular magnet. In the proposed research, we will introduce functionality into our organic component to `turn on' and `turn off' molecular magnetic properties. We propose to do this in three ways: by (a) incorporating a redox active site; or (b) building a redox active organic backbone; or (3) using light to change the conformation of our molecules. These approaches will enable us to induce a switch at the molecular level for our systems. The knowledge that is generated by our proposed research will be used by us and by others to advance the fields of environmental anionic detection and molecular magnetism. Our research group has unique expertise in the analysis of single crystal X-ray structures and magnetism, and combined, we are positioned to provide new insights in structure-function relationships. This environment will provide trainees with excellent opportunities to develop skills that will equip them to contribute to academic, government, and industrial research labs, ensuring that this research program will benefit the larger Canadian community.