TTS APC: Transborylation: A Turnover Strategy for Asymmetric p-Block Catalysis

TTS APC：硼基转移：不对称 p 嵌段催化的周转策略

• 批准号: EP/Y029321/1
• 负责人: Stephen Thomas
• 金额: $ 23.84万
• 依托单位: University of Edinburgh
• 依托单位国家: 英国
• 项目类别: Fellowship
• 财政年份: 2024
• 资助国家: 英国
• 起止时间: 2024 至 无数据
• 项目状态: 未结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FY029321%2F1
• 关键词: TTS; APC; Transborylation; Turnover; Strategy

80% of manufactured chemicals, from plastics to pharmaceuticals, require at least one catalysed-step in their production. Catalysis,particularly industrially, is dominated by the platinum-group metals. These scarce, high toxicity and expensive metals significantly limit sustainably. Their dominance can be attributed to the entrenched understanding and (redox) mechanisms by which metal catalysts undergo turnover, catalyst regeneration. To move beyond (d-block) metal catalysis, new turnover mechanisms are needed and these must be tailored to the wider periodic table. This Fellowship will develop and demonstrate a new turnover mechanism tailored to the p-block and enable sustainable catalysis using p-block elements to be realised.This Fellowship will enable catalysis using transborylation, a redox neutral turnover distinct from metal catalysis. Transborylation will exploit the inherent exchange reactions of p-block elements and introduce control and selectivity to enable directed catalytic turnover. Out proof of principle results have shown transborylation catalysis is possible, but success has been achieved through trial and error. No clear understanding or guiding principles have been established and asymmetric carbon-carbon bond formation is yet to be exploited: the process most required in pharmaceutical and materials development.We will build a fundamental understanding of transborylation across p-block elements and establish a set of guiding principals for exploitation. These principles will then be demonstrated by developing two born-catalysed asymmetric carbon-carbon bond forming reactions. We have chosen a textbook, stoichiometric organoboron reaction (allylation) and a reaction without chemical or biological precedence (doubly reductive ester coupling). Finally we will extend catalysis beyond boron species to the wider p-block. This Fellowship will break the dominance of platinum-group metal catalysis and underpin the sustainable future of chemistry.

从塑料到药物，有80％的制成化学品在其生产中至少需要一个催化阶段。催化，尤其是工业上，由铂群金属主导。这些稀缺，高毒性和昂贵的金属可持续限制。它们的主导地位可以归因于金属催化剂经过营业层，催化剂再生的根深蒂固的理解和（氧化还原）机制。为了超越（D-Block）金属催化，需要新的周转机制，这些机制必须定制在更宽的元素周期表上。该奖学金将开发并展示一种针对P块的新的周转机制，并可以使用P块元素来实现可持续的催化。该研究金将使用Transborylation促进催化，这是一种与金属催化不同的氧化还原中性周转。透射率将利用P块元件的固有交换反应，并引入控制和选择性以实现有向的催化转移。原理结果证明已表明透射率催化是可能的，但是通过反复试验获得了成功。尚未建立明确的理解或指导原则，并且尚未利用不对称的碳 - 碳键形成：药物和材料开发中最需要的过程。我们将建立对跨P块元素传播的基本了解，并建立一系列指导原理。然后，将通过开发两个出生的催化不对称碳碳键形成反应来证明这些原理。我们选择了一本教科书，化学计量有机体反应（烯丙基化）和没有化学或生物学先例的反应（双重还原酯偶联）。最后，我们将将催化范围从硼物种范围内延伸到更广泛的P块。该奖学金将打破铂金属催化的主导地位，并支撑化学的可持续未来。