Small molecule activation and sensing

小分子激活和传感

• 批准号: RGPIN-2014-03970
• 负责人: Song, Datong
• 金额: $ 3.93万
• 依托单位: University of Toronto
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2018
• 资助国家: 加拿大
• 起止时间: 2018-01-01 至 2019-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=665601
• 关键词: Small; molecule; activation; sensing

The proposed research program is focused on the activation and detection of small molecules. * The first objective is to develop fundamentally new and green ways to capture carbon dioxide, which is a potent greenhouse gas and carbon waste from the combustion of all fossil fuels, and to utilize it as sustainable one-carbon feedstock to prepare value-added organic products. In 2013, our group developed a series of compounds (including a metal-free one), which can selectively break one of their own carbon-hydrogen bonds and store one molecule of carbon dioxide in between. We will apply the knowledge gained from this recent breakthrough to design new systems that can selectively break other types of bonds and store carbon dioxide in between. Moreover, we will develop catalytic processes to convert the stored carbon dioxide into organic compounds (such as formate) which have important industrial applications. * The second objective is to solve the mystery of how nature converts atmospheric dinitrogen into ammonia and to learn how to make other nitrogen compounds directly from dinitrogen. We will prepare novel iron compounds that structurally resemble the active site of nitrogenase (nature's enzyme that converts dinitrogen into ammonia) and investigate the reactivity of these compounds toward dinitrogen to deduce the nitrogenase behaviours. One puzzling feature of the nitrogenase activity is the loss of dihydrogen upon dinitrogen binding on an iron centre at the active site. In 2010, our group observed an analogous reactivity when heating a ruthenium (the element right below iron in the periodic table) compound under dinitrogen, i.e., dinitrogen binds with the ruthenium centre with concomitant loss of dihydrogen. Prompted by this analogy, we will further explore the reactivity of the ruthenium-bound dinitrogen, which may provide insight into the reactivity patterns of metal-bound dinitrogen. Information gained from this research will shed light on how nature converts dinitrogen into ammonia and help us harness dinitrogen reactivity to make nitrogen-containing organic compounds directly from the abundant dinitrogen gas from air.* The third objective is to design luminescent sensors for detecting ecotoxins. In 2013, our group developed a selective sensor for DMF vapor, which is responsible for several occupational health problems at leather and synthetic fibre factories, and studied the underlying mechanism. We will apply this knowledge to the design of sensors for detecting nitrate and formaldehyde; the former is a prevalent harmful chemical found worldwide in urban homes and furniture, while the latter is a pollutant in drinking water caused by the overuse of fertilizers. Efforts will also be made to generalize the principle of our sensor design toward the sensing of other environmentally concerned chemicals. The successful outcome will result in portable sensors for the facile detection of pollutants in air and water.* All these projects have positive environmental impacts, and contribute to the advancement of knowledge at both fundamental and practical levels.

提出的研究计划的重点是小分子的激活和检测。 *第一个目标是开发捕获二氧化碳的新方法，这是所有化石燃料的燃烧中有效的温室气和碳废物，并将其用作可持续的单碳原料来准备增值有机产品。在2013年，我们的小组开发了一系列化合物（包括无金属质合质），它们可以选择性地打破自己的一种碳 - 氢键，并在中间储存一个分子的二氧化碳分子。我们将运用从最近的突破中获得的知识来设计新系统，这些系统可以选择性地破坏其他类型的键并在中间存储二氧化碳。此外，我们将开发催化过程，将储存的二氧化碳转换为具有重要工业应用的有机化合物（例如甲状腺）。 *第二个目标是解决大自然如何将大气丁香原转化为氨的奥秘，并学习如何直接从Dinitrogen中制成其他氮化合物。我们将制备新型的铁化合物，从结构上类似于氮酶的活性位点（将二氮转化为氨的酶），并研究这些化合物对二氮的反应性以推断氮酶行为。氮酶活性的一个令人困惑的特征是在活性位点的铁心中心结合二氢二氢因素的丧失。在2010年，我们的小组观察到在二氮下加热丁酸（元素化表中的铁下方的元素）（即元素化表中的铁下方的元素），即二氮与芳基中心结合而伴有二氢损失的二氮中心。在这种类比的提示下，我们将进一步探索氟苯甲部结合的二氮的反应性，这可能会洞悉金属结合的二氮的反应性模式。从这项研究中获得的信息将阐明自然如何将二氮转化为氨，并帮助我们利用Dinitrogen反应性，使含氮的有机化合物直接从空气中的丰富二硝基气体中直接从空气中进行。*第三个目标是设计发光的传感器来检测生态毒素。 2013年，我们的小组开发了DMF Vapor的选择性传感器，该传感器负责皮革和合成纤维工厂的几个职业健康问题，并研究了基本机制。我们将将这些知识应用于传感器的设计，以检测硝酸盐和甲醛。前者是全世界在城市房屋和家具中发现的普遍有害化学物质，而后者是由于肥料过度使用而引起的饮用水中的污染物。还将努力将传感器设计的原理推广到对其他与环境相关的化学物质的感知。成功的结果将导致可容纳空气和水中污染物的便携式传感器。