Applications of Cyclopropenylidene Metal Complexes and Thioureas in Catalysis

我们的研究计划结合了有机合成，计算和物理有机化学，旨在改进催化过程和开发新的催化过程。这些活动提供了对化学反应性、分子结构和键合的机械见解。促进这种兴趣的是催化剂在生产具有医学重要性的天然和非天然化合物、散装材料如聚合物、精细化学品以及来自化石和可再生燃料源的能量中的广泛使用，同时推进更高效和绿色的制造工艺以保护日益减少的资源和保护环境。在未来五年，我们的计划将集中在以下几个方面： (1)我们将开发从钴金属（铜，银，金）衍生的络合物，并将其应用于广泛的有用化学产品。特别感兴趣的将是这些配合物在提供小环中原子的独特排列的反应中的用途，对反应非常沉默的化学键的活化，以及杂环化合物的合成。我们预计，这些配合物将表现出一些有趣的化学性质，我们将通过理论和光谱技术相结合的研究。 (2)我们将开发基于硫脲的氢键催化剂，该催化剂将应用于糖的合成，包括C-糖苷，天然化合物，这些化合物在许多抗肿瘤，抗生素和抗糖尿病（II型）药物中起关键作用。C-糖苷是糖类似物，其区别在于单个原子的细微存在，其合成是重要的，因为它们对代谢的稳定性和在细胞组织中的特定功能。由于C-糖苷在患者的血液和组织中持续时间较长，因此它们在新药设计中很有用。我们预计这一领域的发现将产生深远的成果，直接适用于催化，基础化学理解和药物开发。 除了对反应机制和化学键合的基本见解外，拟议研究的结果将推动有机合成，催化和材料科学领域的发展。我们在一系列金属络合物和硫脲氢键催化剂方面的进展将使新的催化模式成为可能，从而为复杂的天然产物、药物靶标和增值化学品提供有效的合成路线。这项研究还将为制药行业和学术界未来的化学专业人员提供良好的培训。

Our research program combines organic synthesis, computational, and physical organic chemistry directed at the improvement of catalytic processes and the development of new ones. These activities provide mechanistic insight into chemical reactivity, molecular structure, and bonding. Fueling this interest is the widespread use of catalysis in the production of medicinally important natural and unnatural compounds, bulk materials such as polymers, fine chemicals, and energy from both fossil and renewable fuel sources, while advancing more efficient and green manufacturing processes to preserve diminishing resources and protect the environment. Over the next five years our program will focus on the following: (1) We will develop complexes derived from coinage metals (copper, silver, gold) and apply these to a broad spectrum of useful chemical products. Of specific interest will be the use of these complexes in reactions providing unique arrangements of atoms in small rings, activation of chemical bonds that are very reticent to react, and the synthesis of heterocyclic compounds. We anticipate that these complexes will exhibit a number of interesting chemical properties, which we will investigate through the combination of theoretical and spectroscopic techniques. (2) We will develop thiourea-based hydrogen bond catalyst that will be applied to the synthesis of sugars, including C-glycosides, compounds from nature that serve as key motifs in numerous antitumor, antibiotic, and antidiabetic (type II) agents. The synthesis of C-glycosides, which are sugar analogs differing by the subtle presence of a single atom, is of importance because of their stability to metabolism and specific function in cellular tissues. Because C-glycosides last longer in the blood and tissues of patients, they are useful in the design of new drugs. We project this area of discovery will have far-reaching outcomes directly applicable to catalysis, basic chemical understanding, and drug development. In addition to fundamental insight into reaction mechanisms and chemical bonding, the outcome of the proposed research will advance the fields of organic synthesis, catalysis, and material science. Our advancement of an array of metal complexes and thiourea hydrogen bond catalysts will enable new modes of catalysis allowing for efficient synthetic routes to complex natural products, pharmaceutical targets, and value-added chemicals. This research will also provide excellent training for future chemistry professionals both in the pharmaceutical industry and in academia.