sigma-Aromatic Actinide-Actinide Bonding: A New Frontier in f-Block Chemistry
sigma-Aromatic Actinide-Actinide Bonding: A New Frontier in f-Block Chemistry
批准号:
EP/W029057/1
负责人:
Stephen Liddle
金额:
$114.41万
依托单位:
依托单位国家:
英国
项目类别:
Research Grant
财政年份:
2022
资助国家:
英国
项目状态:
未结题
起止时间:
2022 至 --
中文摘要
元素周期表主要由金属组成。因此,金属-金属键合是一个广阔的新兴领域,它是推动我们对结构、成键、反应性和磁性理解的阶段性变化的基础。在177年的时间里,S、p和d块产生了无数例行公事的不同金属-金属键合图案的例子。相比之下,作为合成AN化学的首要目标之一,可分离的鳗系元素(AN-AN)键在那段时间里一直难以捉摸,这排除了对反应模式的评估,而反应模式是理解金属-金属键的核心原则。这个大胆的项目旨在利用我们最近发现的分子可分离的钍-钍键(自然2021,598,72-75),它描述了令人惊讶的西格玛-芳香键,以记录元素周期表中的主量子数6和7行以及多电子小分子的激活反应性。在我们初步结果的基础上,这个项目试图扩大AN-AN络合物的范围,确定它们的反应趋势,并使用一系列全面的实验和理论表征技术来探索它们的电子结构和物理化学性质。这将涉及广泛的项目合作伙伴以及国家和国际研究机构,使之成为一种连贯和相互交错的办法。这项研究对核能部门具有重要的战略意义,因为它将保留一名熟练的ECR,并在英国一个已知的技能短缺领域培训两名新的ECR,我们将与利益相关者一起开发处理放射性元素的“最佳实践”方法,从而促进学术界的知识转移:行业接口。通过研究项目中概述的化合物,将开发分析技术的新应用,由此产生的方法进步将在内部发展这些学科的能力和健康,而且更广泛地说,因为这些技术涉及设施和研究人员,这些设施和研究人员在许多其他领域开展工作,可以从新工作方式的转移中受益。这个项目是适时开发的,我们的初步结果表明,这项工作是可以实现的,也是有影响的。因此,我们要求与拟议工作的范围和雄心相称的资金来开发这一有希望的领域,以利用我们的突破,保持在这一新创建和令人兴奋的领域的国际前沿,并产生对AN-化学具有国际意义的成果。
英文摘要
The Periodic Table is mainly composed of metals. Thus, metal-metal bonding is a vast burgeoning field that is fundamental to driving step-changes in our understanding of structure, bonding, reactivity, and magnetism. Over 177 years the s-, p-, and d-blocks have produced numerous routinely isolable examples of varied metal-metal bonding motifs. In contrast, isolable actinide-actinide (An-An) bonding, one of the top goals of synthetic An-chemistry, has remained elusive in all that time, precluding assessment of reactivity patterns that are a central tenet of understanding metal-metal bonding. This adventurous project aims to exploit our recent discovery of molecular isolable thorium-thorium bonding (Nature 2021, 598, 72-75), which describes surprising sigma-aromatic bonding to record principal quantum number 6 and 7th row of the Periodic Table and multi-electron small molecule activation reactivity. Building on our preliminary result, this project seeks to expand the range of An-An complexes, determine their reactivity trends, and probe their electronic structure and physicochemical properties using a comprehensive range of experimental and theoretical characterisation techniques. This will involve a wide range of project partners and national and international research facilities brought together into a cohesive and interleaved approach. This research is strategically important with respect to the nuclear sector, as it will retain a skilled ECR and train two new ones in a known UK skills-shortage area, and together with stakeholders we will develop 'best practice' methods for handling radioactive elements, thus promoting knowledge transfer at the academia:industry interface. By studying the compounds outlined in the project, new applications of analytical techniques will be developed, and the resulting methodological advances will develop the capability and health of those disciplines in-house, and also more broadly because those techniques involve facilities and researchers that work across many other areas that could benefit from the transfer of new working ways. This project is timely to develop and our preliminary results show the work is achievable and impactful. Thus, we request funds commensurate with the scope and ambition of the proposed work to develop this promising area in order to capitalise on our breakthrough, stay at the international forefront of this newly created and exciting field, and generate results of international significance to An-chemistry.
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