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In situ studies of materials for high temperature CO2 capture and storage

机译：高温CO2捕集与封存材料的原位研究

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Carbon capture and storage ( CCS) offers a possible solution to curb the CO2 emissions from stationary sources in the coming decades, considering the delays in shifting energy generation to carbon neutral sources such as wind, solar and biomass. The most mature technology for post-combustion capture uses a liquid sorbent, amine scrubbing. However, with the existing technology, a large amount of heat is required for the regeneration of the liquid sorbent, which introduces a substantial energy penalty. The use of alternative sorbents for CO2 capture, such as the CaO-CaCO3 system, has been investigated extensively in recent years. However there are significant problems associated with the use of CaO based sorbents, the most challenging one being the deactivation of the sorbent material. When sorbents such as natural limestone are used, the capture capacity of the solid sorbent can fall by as much as 90 mol% after the first 20 carbonation-regeneration cycles. In this study a variety of techniques were employed to understand better the cause of this deterioration from both a structural and morphological standpoint. X-ray and neutron PDF studies were employed to understand better the local surface and interfacial structures formed upon reaction, finding that after carbonation the surface roughness is decreased for CaO. In situ synchrotron X-ray diffraction studies showed that carbonation with added steam leads to a faster and more complete conversion of CaO than under conditions without steam, as evidenced by the phases seen at different depths within the sample. Finally, in situ X- ray tomography experiments were employed to track the morphological changes in the sorbents during carbonation, observing directly the reduction in porosity and increase in tortuosity of the pore network over multiple calcination reactions.
机译：考虑到将能源发电转移到碳中性能源（例如风能，太阳能和生物质能）方面的延迟，碳捕集与封存（CCS）提供了一种可能的解决方案，可在未来数十年内抑制固定来源的CO2排放。燃烧后捕集的最成熟技术是使用液体吸附剂，胺洗涤。然而，利用现有技术，液体吸附剂的再生需要大量的热量，这带来了巨大的能量损失。近年来，已经广泛研究了使用替代吸附剂来捕获二氧化碳，例如CaO-CaCO3系统。然而，与基于CaO的吸附剂的使用相关的重大问题，最具挑战性的一个是吸附剂材料的失活。当使用吸附剂（例如天然石灰石）时，在最初的20个碳酸再生循环之后，固体吸附剂的捕获能力可能会下降90 mol％。在这项研究中，采用了多种技术从结构和形态的角度更好地了解这种劣化的原因。 X射线和中子PDF研究被用来更好地了解反应后形成的局部表面和界面结构，发现碳酸化后CaO的表面粗糙度降低了。原位同步加速器X射线衍射研究表明，与在没有蒸汽的条件下相比，在添加蒸汽的情况下碳酸化导致CaO的转化更快，更完全，这在样品中不同深度处观察到的相证明了这一点。最后，采用原位X射线断层扫描实验跟踪碳化过程中吸附剂的形态变化，直接观察孔隙率的降低和多次煅烧反应后孔隙网络的曲折度的增加。

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