Energy and the Physical Sciences: Advanced materials for thermo-chemical oxygen storage and production

在这项提议中，我们打算采取一种新的方法来解决涉及反应和/或分离的问题。我们采用高温化学环的思想，通过开发和研究能够作为固态氧载体的新型先进材料，将其应用于中温。这种方法将适用于广泛的过程；在这里，我们打算通过含氧物和氧气生产的自热重整来证明其有效性。更先进的材料开辟了新的应用领域，因为能够定制它们的化学和结构来改变氧转移的热力学和动力学。我们还将在许多范围内开展工作，将材料的基本化学与其氧转移特性联系起来，促进合理的材料设计方法。基础化学和过程工程之间的这种反馈是这项建议的一个独特特点。将研究简单金属氧化物和混合物，以及混合金属氧化物阴离子导电材料，如LSCF(钙钛矿)和镍酸镧/钴(Ruddlesdon Popper结构)，以确定它们在供氧体/化学循环过程中的有效性。后一种材料为材料设计提供了一个起点，因为它们可以被其他阳离子取代，从而允许调整其氧源/氧汇的化学势。同时，我们还将利用可公开获得的数据库中的能量学，并通过使用DFT计算的有针对性的第一原理，筛选适合于重整和制氧过程的新材料。

In this proposal we intend to take a novel approach to problems involving reaction and/or separation. We adopt the ideas of high temperature chemical looping and apply them at intermediate temperature by developing and investigating new, advanced materials capable of acting as solid state oxygen carriers. This approach would be applicable to a wide range of processes; here we intend to begin by demonstrating its validity through autothermal reforming of oxygenates and oxygen production. More advanced materials open up new areas of application owing to the ability to tailor their chemistry and structure to change both the thermodynamics and kinetics of oxygen transfer. We will also work across many scales to link the fundamental chemistry of the materials to their oxygen transfer characteristics, facilitating a rational approach to materials design. This feedback between the fundamental chemistry and the process engineering is a unique feature of this proposal. Simple metal oxides and mixtures, and mixed metal oxide anion conducting materials, e.g. LSCF (a perovskite) and lanthanum-nickelates/cobaltates (a Ruddlesdon Popper structure), will be examined to determine their usefulness in oxygen donor/chemical looping processes. The latter materials offer a starting point for material design since they are amenable to substitution with other cations allowing the chemical potential of their oxygen sources/sinks to be tuned. In parallel we will also screen, making use of energetics available from publicly available data bases and via targeted first principles using DFT calculations, for novel materials suitable for reforming and oxygen production processes.