Functional Metal-Nitrogen-Hydrogen Systems

化学是现代许多重大技术变革的核心。从能源密集但对环境有害的化石燃料的紧急过渡为化学提出了一个新的重大挑战，其核心是与能源转换，分配和利用相关的材料设计。特别是太阳能和风能的迅速发展，将需要在家庭电力、交通和电网管理等不同应用中使用大规模的能量存储，涵盖广泛的能量、功率和存储时间。为了应对这一挑战，我们必须利用现有技术，同时开发具有增强性能的新材料。该研究金申请中包含的研究方案详细说明了开发一种新的无机金属-氮-氢（M-N-H）材料家族的计划，重点是它们在可持续能源储存方面的应用。该项目的核心是一个合成计划，旨在显著扩大M-N-H材料的范围，除了这些第一个例子之外，我们还讨论了具有更广泛的化学键合类型和金属的体系。M-N-H材料的应用主要局限于第I族和第II族金属的酰胺和酰亚胺（含NH 2和NH 2的无机盐）在轻质储氢材料中的应用。最近，这些相同的材料已被鉴定为有效的氨分解催化剂，并且与基于水的复合催化剂的增强的氨合成活性有关。氨越来越被认为是一种可行的高能量密度燃料和氢载体，M-N-H材料的催化活性可能有助于促进其使用。因此，该研究金的一个主题将是扩大数量相对较少的材料的催化活性测试。M-N-H新材料的筛选不仅可以开发出更高活性的催化剂，而且可以更全面地了解其催化作用的性质。许多功能材料都是基于氧化物的，而性能的变化来自于氧化物材料中阳离子排列的变化。酰亚胺阴离子类似于氧化物，因此提供了一种创造类似材料的途径。例如，氧化锂和酰亚胺锂是同构的，然而酰亚胺锂显示出与氧化物相比显著增强的离子电导率。该计划的这一部分将试图阐明酰亚胺和氧化物之间的关系，并使用这一原则作为指导设计新的酰亚胺基功能材料。特别地，将追求具有高离子电导率和电化学活性组分（例如阴极材料）的酰亚胺的合成，目标是开发概念酰亚胺电池材料。其目的是为M-N-H家族的基础化学提供新的见解，并说明储能材料设计的新方法。

Chemistry is at the heart of many of the great technological transformations of the modern era. The urgent transition away from energy-dense but environmentally-damaging fossil fuels presents a new grand challenge for chemistry, centred on the design of materials associated with the conversion, distribution and utilisation of energy. In particular, the rapid expansion of solar and wind power will necessitate the use of large-scale energy storage, spanning wide ranges of energy, power and storage duration in diverse applications including domestic power, transportation and grid management.In order to meet this challenge, we must leverage existing technology while simultaneously developing new materials with enhanced properties. The research programme contained within this Fellowship application details a plan to develop a new family of inorganic metal-nitrogen-hydrogen (M-N-H) materials, with an emphasis on their application to sustainable energy storage. At the core of this project is a synthetic programme which aims to significantly expand the range of M-N-H materials, moving beyond these first examples to systems which display a wider range chemical bonding types and metals.Consideration of the application of M-N-H materials has been largely restricted to the Group I and II metal amides and imides (NH2- and NH2- bearing inorganic salts) in the context of lightweight hydrogen storage materials. More recently, these same materials have been identified as effective ammonia decomposition catalysts, and have been implicated in the enhanced ammonia synthesis activity of hydride-based composite catalysts. Ammonia is increasingly considered as a viable high energy density fuel and hydrogen carrier, and the catalytic activity of M-N-H materials may help promote its use. One theme of this fellowship will therefore be the expansion of the relatively small number of materials have been tested for their catalytic activity. Screening of the new M-N-H materials would not only result in the development of more active catalysts, but also a more complete understanding of the properties which govern their catalytic action.Many functional materials are based on oxides, and property variation comes from varying the array of cations in the oxide material. Imide anions are similar to oxide, and so offer a path to creating analogous materials. For example, lithium oxide and lithium imide are isostructural, yet lithium imide shows ionic conductivity which is dramatically enhanced compared to the oxide. This part of the programme will seek to elucidate the relationship between imides and oxides, and to use this principle as a guide for the design of new imide-based functional materials. In particular, synthesis of imides with high ionic conductivity and electrochemically-active components (e.g. cathode materials) will be pursued with the goal of developing a concept imide battery material. The aim is to provide new insights into the fundamental chemistry of the M-N-H family and illustrate new approaches for the design of energy storage materials.