Theoretical and Experimental Studies of Metal Catalysed Reactions and Boron-Containing Optical Materials

金属催化反应及含硼光学材料的理论与实验研究

• 批准号: EP/H01120X/1
• 负责人: Todd Marder
• 金额: $ 6.7万
• 依托单位: Durham University
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2009
• 资助国家: 英国
• 起止时间: 2009 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FH01120X%2F1
• 关键词: Theoretical; Experimental; Studies; Metal; Catalysed

Catalysis of organic reactions, especially those involving carbon-carbon bond formation, is an important area of chemistry as such reactions are used in almost all organic syntheses including the manufacture of pharmaceuticals and agrochemicals, liquid crystals, and conjugated materials for applications in flat-screen displays. In addition to developing new catalyst systems for the above reactions, we are also developing new catalytic routes to organoboronate esters which are key synthetic intermediates in many of these reactions including homocoupling and cross-coupling reactions to form carbon-carbon and carbon-heteroatom bonds. These reactions also have applications in the rapid synthesis of organic compounds widely used in industry, for example, for drug and agrochemical discovery, in addition to large-scale manufacturing. We employ a combined approach to developing catalysts and catalytic process which incorporates experimental studies as well as theoretical studies, the latter providing an improved understanding of how the reactions work, which feeds back into our experimental programmes thus assisting in the development of catalysts by design. The ongoing, highly productive collaboration with theoretician Prof. Z. Lin (HKUST) has proven invaluable in this regard, and the applicant wishes to improve his own ability to carry out such theoretical studies. Experimental studies on catalyst development are ongoing with Profs. Z. Yang (Peking University) and A. Lei (Wuhan University) which have already led to new catalysts for several important carbon-carbon bond forming reactions.Another area of chemistry which is very active is the development of new molecules with useful optical properties. Such compounds absorb and emit light or emit light in response to the application of electricity, and can be used in many applications including high resolution imaging (in 3 dimensions) in biological systems (for example, two-photon absorbing compounds allow for a high degree of spatial resolution in the depth dimension), as well as in Organic Light Emitting Diodes (OLEDs), the latter being important for the next generation of flat-screen displays. We are working (together with Profs. W.-Y. Wong at Hong Kong Baptist University, Z. Xi at Peking University, and Z. Liu at Shandong University) on the development of new organic and organometallic compounds containing boron which exhibit enhanced optical properties for the above applications.Finally, we are developing small organic molecules which are stable to ambient conditions (e.g., air and light) and can be used as alternatives to the naturally occurring All-Trans Retinoic Acid (ATRA, a metabolite of Vitamin A) to trigger the differentiation of stem cells. ATRA suffers from its instability to air and especially light, causing problems in practical applications in cell culture, as the isomers formed upon exposure to normal laboratory light exhibit different biological activity. The new molecules we are developing are stable, allowing, e.g., the differentiation of stem cells to give rise to neurons (nerve cells) only, as opposed to mixtures of cell types. This work involves collaboration with organic chemists and biologists in Durham, as well as SMEs specializing in enabling stem cell technologies (Reinnervate Ltd.) and in synthesis of pharmaceutical intermediates (High force Research Ltd.). We plan to expand this collaboration to include Prof. Z. Yang (Laboratory for Chemical Genomics at the Shenzhen Graduate School of Peking University, where he is Changjiang Professor and Dean of the College of Chemical Biology and BioTechnology) as his research groups in both Beijing and Shenzhen have expertise in the synthesis of related biologically active compounds which we would like to study in our processes, and also access to a special laboratory containing over 1000 trangenic zebra fish which can be used to study rapidly the developmental effects of the retinoids we are synthesizing.

有机反应的催化，特别是涉及碳-碳键形成的反应，是化学的一个重要领域，因为此类反应几乎用于所有有机合成，包括药物和农用化学品、液晶以及用于平板显示器的共轭材料的制造。除了为上述反应开发新的催化剂体系外，我们还在开发有机硼酸酯的新催化路线，有机硼酸酯是许多此类反应的关键合成中间体，包括形成碳-碳和碳-杂原子键的自偶联和交叉偶联反应。除了大规模制造之外，这些反应还可以应用于工业中广泛使用的有机化合物的快速合成，例如药物和农用化学品的发现。我们采用组合方法来开发催化剂和催化过程，其中结合了实验研究和理论研究，后者提供了对反应如何工作的更好的理解，这反馈到我们的实验计划中，从而有助于通过设计开发催化剂。事实证明，与理论家林中正教授（香港科技大学）正在进行的、富有成效的合作在这方面是非常宝贵的，申请人希望提高自己进行此类理论研究的能力。教授们正在进行催化剂开发的实验研究。 Z. Yang（北京大学）和A. Lei（武汉大学）已经为几个重要的碳-碳键形成反应开发了新的催化剂。化学的另一个非常活跃的领域是开发具有有用光学性质的新分子。此类化合物吸收并发射光或响应于电力的施加而发射光，并且可用于许多应用，包括生物系统中的高分辨率成像（3维）（例如，双光子吸收化合物允许在深度维度上实现高度的空间分辨率）以及有机发光二极管（OLED），后者对于下一代平板屏幕非常重要 显示。我们（与香港浸会大学的 W.-Y. Wong 教授、北京大学的 Z. Xi 教授和山东大学的 Z. Liu 教授一起）致力于开发新型含硼有机和有机金属化合物，这些化合物在上述应用中表现出增强的光学性能。最后，我们正在开发对环境条件（例如空气和光）稳定的有机小分子，可用作 天然存在的全反式视黄酸（ATRA，维生素 A 的代谢产物）的替代品，可触发干细胞的分化。 ATRA 对空气尤其是光不稳定，在细胞培养的实际应用中造成问题，因为暴露于正常实验室光线时形成的异构体表现出不同的生物活性。我们正在开发的新分子是稳定的，例如，允许干细胞分化仅产生神经元（神经细胞），而不是细胞类型的混合物。这项工作涉及与达勒姆有机化学家和生物学家以及专门从事干细胞技术（Reinnervate Ltd.）和药物中间体合成（High Force Research Ltd.）的中小企业的合作。我们计划扩大这一合作范围，将杨正教授（北京大学深圳研究生院化学基因组学实验室，长江教授兼化学生物学与生物技术学院院长）纳入其中，因为他在北京和深圳的研究小组在合成相关生物活性化合物方面拥有专业知识，我们希望在我们的工艺中研究这些化合物，并且还可以使用包含以下内容的特殊实验室： 超过 1000 条转基因斑马鱼，可用于快速研究我们正在合成的类视黄醇的发育效应。