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造成破坏的化石燃料的紧迫转型，对化学提出了新的重大挑战，重点是与能源转换、分配和利用相关的材料的设计。特别是，太阳能和风能的快速发展将需要使用大规模的储能，在包括家庭电力、交通运输和电网管理在内的不同应用中，跨越广泛的能量、电力和储存时间。为了应对这一挑战，我们必须利用现有技术，同时开发性能更高的新材料。该研究金申请中的研究方案详细说明了一项开发新型无机金属-氮-氢(M-N-H)材料家族的计划，重点是将其应用于可持续能源储存。该项目的核心是一项合成计划，旨在显著扩大M-N-H材料的范围，超越这些第一个例子，转向显示更广泛的化学键类型和金属的系统。在轻量级储氢材料的背景下，M-N-H材料的应用在很大程度上被限制在I和II族金属酰胺和亚胺(含NH2和NH2的无机盐)的范围内。最近，这些相同的材料被确定为有效的氨分解催化剂，并被用于提高氢化物基复合催化剂的氨合成活性。氨越来越被认为是一种可行的高能量密度燃料和氢载体，而M-N-H材料的催化活性可能有助于促进其应用。因此，这一研究金的一个主题将是扩大经过催化活性测试的相对较少的材料。筛选新的M-N-H材料不仅可以开发出活性更高的催化剂，还可以更全面地了解它们的催化性能。许多功能材料都是以氧化物为基础的，性能的变化来自于氧化物材料中阳离子的排列。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，锂氧化物和锂酰亚胺是同构的，但锂酰亚胺表现出比氧化物显著增强的离子导电性。该方案的这一部分将力求阐明酰亚胺和氧化物之间的关系，并将这一原则作为设计新的亚胺类功能材料的指南。特别是，具有高离子导电性和电化学活性成分(如正极材料)的酰亚胺的合成将以开发概念亚胺电池材料为目标。其目的是为M-N-H系列的基本化学提供新的见解，并说明设计储能材料的新方法。

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.