Chemical Speciation using Advanced Spectroscopic Methods

使用先进的光谱方法进行化学形态分析

• 批准号: RGPIN-2016-04546
• 负责人: Jalilehvand, Farideh
• 金额: $ 1.82万
• 依托单位: University of Calgary
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2019
• 资助国家: 加拿大
• 起止时间: 2019-01-01 至 2020-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=680358
• 关键词: Chemical; Speciation; using; Advanced; Spectroscopic

Metal ions are extensively used in industry with applications in agriculture, catalysis, batteries, etc. They also have diverse biomedical applications with anticancer, radiopharmaceutical or antibacterial activities. Since the discovery of cis-platin (cis-[Pt(NH3)2Cl2]) in the 1970s as the first metal-based anticancer chemotherapeutic agent, many research activities have focused on developing new metal complexes with anticancer properties. The goal has been to identify chemical reagents that have a higher selectivity toward cancerous cells and less toxic side effects compared with cis-platin.*** Bimetallic complexes of rhodium(2+), ruthenium(2+/3+) and rhenium(3+) ions, with (O,O) or (O,N)-donor species bridging between the two metal ions and a (semi) paddle wheel structure, are promising metal-based antitumor active compounds, with DNA as their primary target. However, these are not clinically in use mainly because their interactions with other biomolecules are not fully understood. We will therefore investigate the reaction products of these bimetallic complexes with selected amino acids, including histidine, methionine, cysteine and its derivatives, as well as the tri-peptide glutathione, as models for interactions of these bimetallic compounds with proteins and enzymes. For this purpose, we will use the X-ray region of synchrotron light, which is more than a million times brighter than the sun and is produced at synchrotron facilities around the world, including the Canadian Light Source (CLS). A state-of-the-art microscopy technique with a synchrotron light source will be used to monitor the cellular uptake of these antitumor active complexes and map the intracellular distribution of elements, such as rhodium, rhenium, ruthenium, sulfur and phosphorus, in each cell. This knowledge will help to understand the fate of this class of antitumor-active compounds as they enter the cell. *** We are also interested in a new generation of lithium ion batteries, in which ionic liquids (ILs) are used as non-flammable electrolytes and lithium (Li) metal as the anode. Due to the highly reactive surface of Li, the IL is decomposed at its surface and a solid electrolyte interphase (SEI) is formed. Depending on the type of IL used, the SEI can be “beneficial”, allowing extended cycling of the battery, or “detrimental”, impending the battery performance. We will use state-of-the-art synchrotron-based techniques to identify the chemical species formed in the SEI on the surface of Li electrodes.*** During this research program, several graduate and undergraduate students will gain experience in using a wide range of spectroscopic techniques, as applied to both biomedical and clean energy applications. Another important purpose of this research is to promote synchrotron science in Canada and to train future users of the CLS facility in Saskatoon.*****

金属离子广泛应用于工业，在农业，催化，电池等方面的应用，它们还具有抗癌，放射性药物或抗菌活性的各种生物医学应用。自20世纪70年代发现顺铂（cis-[Pt（NH3）2Cl 2]）作为第一种基于金属的抗癌化疗剂以来，许多研究活动都集中在开发具有抗癌特性的新金属配合物上。目标是确定与顺铂相比对癌细胞具有更高选择性且毒副作用更小的化学试剂。 铑（2+）、钌（2+/3+）和钌（3+）离子的双金属配合物，在两个金属离子之间有（O，O）或（O，N）-供体物种桥接，具有（半）桨轮结构，是一类很有前途的金属基抗肿瘤活性化合物，其主要靶点是DNA。然而，这些没有在临床上使用，主要是因为它们与其他生物分子的相互作用尚未完全了解。因此，我们将研究这些复合物与选定的氨基酸，包括组氨酸，蛋氨酸，半胱氨酸及其衍生物，以及三肽谷胱甘肽的反应产物，作为这些复合物与蛋白质和酶的相互作用的模型。为此，我们将使用同步加速器光的X射线区域，它比太阳亮100多万倍，并在世界各地的同步加速器设施中产生，包括加拿大光源（CLS）。一个国家的最先进的显微镜技术与同步加速器光源将被用来监测这些抗肿瘤活性复合物的细胞摄取和映射的元素，如铑，钌，硫和磷，在每个细胞的细胞内分布。这些知识将有助于了解这类抗肿瘤活性化合物进入细胞后的命运。*** 我们还对新一代锂离子电池感兴趣，其中离子液体（IL）用作不可燃电解质，锂（Li）金属用作阳极。由于Li的高反应性表面，IL在其表面分解并形成固体电解质中间相（SEI）。根据所使用的IL的类型，SEI可以是“有益的”，允许电池的延长循环，或者是“有害的”，影响电池性能。我们将使用最先进的基于同步加速器的技术来识别在锂电极表面上的SEI中形成的化学物质。 在这项研究计划中，一些研究生和本科生将获得使用广泛的光谱技术的经验，适用于生物医学和清洁能源应用。这项研究的另一个重要目的是促进加拿大的同步加速器科学，并培训萨斯卡通CLS设施的未来用户。