Sustainable Alkaline Earth-derived systems for multi-component coupling chemistry, and the exploration of fundamental molecular beryllium systems

碱土金属在两个关键方面被认为是重要的：较重的元素，特别是Mg和Ca，是我们星球上最丰富的两种金属，因此在可持续催化系统中是非常有前途的中心反应位点。相反，最轻的碱土元素Be的化学性质仍然是周期表中所有非放射性金属中研究最少的，尽管它具有独特的性质，例如具有所有金属离子中最小的离子半径，以及伴随的高极化性质。本项目旨在解决这些矛盾点。高丰度的Mg和Ca代表了开发真正良性催化体系的关键候选物。迄今为止，这些元素已被用于许多催化转化，这些催化转化曾经是过渡金属的专有领域，主要涉及到不饱和键（例如亚胺，烯烃）的加成反应（例如氢化硅烷化，氢化）。我们的目标是将这种碱土金属催化扩展到更具挑战性的多组分偶联反应，这些反应仍然是过渡金属的领域。通过明确的化学计量反应性研究，我们将开发由镁和钙催化的烯烃羰基化过程，由硅和硼羰基化反应框架，不仅映射这些金属的新型催化过程，而且确实扩展了烯烃官能化化学的稀有形式。此外，我们将同时开发Be的相关化学计量化学，以彻底增加我们对这种特殊元素分子物种反应能力的了解。这将集中在氢化物和烷基络合物的反应性上，以形成与较重的第2族元素以及周期表中所有金属的已建立的化学进行比较的基础。鉴于在过去15年中第2族金属的低价化学的迷人发展，我们的目标还包括获得高度追求的BeI系统，在主族化学中开辟一个新的子领域。总的来说，该项目将彻底发展我们对第2族金属的基本理解，并建立一套新的可持续催化剂，以应对我们今天面临的一些最大的合成挑战。

The Alkaline Earth metals can be considered significant in two key respects: the heavier elements, specifically Mg and Ca, are two of the most abundant metals on our planet, and thus stand as highly promising central reactive sites in sustainable catalytic systems. Conversely, the chemistry of the lightest Alkaline Earth element, Be, remains the least studied amongst all non-radioactive metals of the periodic table, despite its unique properties such as having the smallest ionic radius of all metal ions, and a concomitantly high polarizing nature. This project aims to address these contrasting points. The highly abundant Mg and Ca represent key candidates for the development of truly benign catalytic systems. To date, these elements have been utilized in a number of catalytic transformations which were once the exclusive domain of transition metals, largely regarding addition reactions (e.g. hydrosilylation, hydrogenation) to unsaturated bonds (e.g. imines, alkenes). We aim to extend such Alkaline Earth metal catalysis towards more challenging multicomponent coupling reactions which remain the domain of transition metals. Through well-defined stoichiometric reactivity studies, we will develop alkene carbonylation processes catalyzed by Mg and Ca, framed by sila- and bora-carbonylation reactions, mapping not only a novel catalytic process for these metals, but indeed expanding what is already a rare form of alkene functionalistion chemistry. In addition, we will simultaneously develop related stoichiometric chemistry of Be, to thoroughly increase our knowledge of the reactive capacity of molecular species of this peculiar element. This will focus on the reactivity of hydride and alkyl complexes, to form a basis for comparison to well established chemistry of the heavier group 2 elements, and indeed that of all metals of the periodic table. Given fascinating developments in the low-valent chemistry of the group 2 metals over the past 15 years, we also aim to access highly sought BeI systems, opening a new sub-field in main group chemistry. As a whole, this project will thus thoroughly develop both our fundamental understanding of the group 2 metals, as well as establishing a new set of sustainable catalysts to tackle some of the greatest synthetic challenges we face today.