Interaction of Nitrogen and Sulfur Species with Oxygen Carriers in Chemical Looping with Oxygen Uncoupling

1606874 -Padak化学循环是碳捕获的一种有前途的策略。在化学链氧解偶联（CLOU）过程中，燃烧过程所需的氧气从一种称为氧载体的金属氧化物中释放出来，消除了空气和燃料之间的直接接触，使二氧化碳容易分离。所提出的工作的目的是调查氮和硫物种与氧载体材料采用各种实验技术以及分子建模的相互作用。这项研究将对未来建造的化学循环工厂产生影响，因为它将提供对CLOU过程中污染物形成的基本了解。如果根据排放水平和条例需要在封存之前对二氧化碳流进行处理，这种理解将有助于排放控制技术的设计。该项目将产生的实验数据将提供对这些污染物对氧载体活性的影响的深入了解，这将有助于设计未来的氧载体材料，该材料将持续许多氧化还原循环，从而降低材料的成本。然而，对于氧载体表面上发生的非均相化学，特别是对于与杂质的相互作用，缺乏基本的理解。在拟议的工作中，铜和锰基氧载体和载体材料的各种组合将在CLOU条件下进行测试，同时暴露于氮和硫物质，以揭示氧载体表面上发生的非均相反应。氧载体表面也将使用密度泛函理论进行模拟，并确定反应途径。通过采用实验室规模的实验和理论模拟，该项目将提供一个基本的了解NOx（氮氧化物）和SOx（硫氧化物）的形成机制，具体到CLOU过程。

1606874 - PadakChemical looping is one of the promising strategies for carbon capture. In the chemical looping oxygen uncoupling (CLOU) process, the oxygen necessary for the combustion process is released from a metal oxide, called the oxygen carrier, eliminating the direct contact between air and fuel, causing carbon dioxide to be easily separated. The objective of the proposed work is to investigate the interaction of nitrogen and sulfur species with the oxygen carrier material employing various experimental techniques as well as molecular modeling. This research will create an impact on the chemical looping plants that will be built in the future, in the sense that it will provide a fundamental understanding of the pollutant formation during the CLOU process. This understanding would aid in the design of emission control technologies, if a treatment of the carbon dioxide stream is required prior to sequestration depending on the emission levels and regulations. Experimental data that will be produced from this project will provide insight into the effect of such pollutants on the activity of the oxygen carrier, which would help the design of future oxygen carrier materials that would last for many oxidation reduction cycles, thus reducing the cost of the materials.There has been a great effort in the discovery of oxygen carrier materials that are suitable for chemical looping applications; however, there is a lack of a fundamental understanding of the heterogeneous chemistry occurring on the oxygen carrier surface, especially for the interactions with impurities. In the proposed work, various combinations of copper and manganese-based oxygen carrier and support materials will be tested under CLOU conditions while being exposed to nitrogen and sulfur species to shed light into the heterogeneous reactions taking place on the oxygen carrier surface. The oxygen carrier surfaces will also be simulated using density functional theory and the reaction pathways will be determined. By employing bench-scale experiments and theoretical simulations, this project will provide a fundamental understanding of NOx (nitrogen oxides) and SOx (sulfur oxides) formation mechanisms specific to the CLOU process.