Department of Physical, Chemical, and Natural Systems , Universidad Pablo de Olavide , Ctra. Utrera km 1 , 41013 Seville , Spain.
DIFFER, Dutch Institute for Fundamental Energy Research , De Zaale 20 , 5612 AJ Eindhoven , The Netherlands.
ACS Appl Mater Interfaces. 2018 Jun 20;10(24):20512-20520. doi: 10.1021/acsami.8b04507. Epub 2018 Jun 5.
Carbon dioxide release has become an important global issue due to the significant and continuous rise in atmospheric CO concentrations and the depletion of carbon-based energy resources. Plasmolysis is a very energy-efficient process for reintroducing CO into energy and chemical cycles by converting CO into CO and O utilizing renewable electricity. The bottleneck of the process is that CO remains mixed with O and residual CO. Therefore, efficient gas separation and recuperation are essential for obtaining pure CO, which, via water gas shift and Fischer-Tropsch reactions, can lead to the production of CO-neutral fuels. The idea behind this work is to provide a separation mechanism based on zeolites to optimize the separation of carbon dioxide, carbon monoxide, and oxygen under mild operational conditions. To achieve this goal, we performed a thorough screening of available zeolites based on topology and adsorptive properties using molecular simulation and ideal adsorption solution theory. FAU, BRE, and MTW are identified as suitable topologies for these separation processes. FAU can be used for the separation of carbon dioxide from carbon monoxide and oxygen and BRE or MTW for the separation of carbon monoxide from oxygen. These results are reinforced by pressure swing adsorption simulations at room temperature combining adsorption columns with pure silica FAU zeolite and zeolite BRE at a Si/Al ratio of 3. These zeolites have the added advantage of being commercially available.
由于大气 CO 浓度的显著持续上升和碳基能源资源的枯竭，二氧化碳的释放已成为一个重要的全球问题。通过利用可再生电力将 CO 转化为 CO 和 O，将 CO 重新引入能源和化学循环是一种非常节能的过程。该过程的瓶颈在于 CO 仍然与 O 和残余 CO 混合。因此，高效的气体分离和回收对于获得纯 CO 至关重要，通过水煤气变换和费托反应，可以生产出 CO 中性燃料。这项工作的思路是提供一种基于沸石的分离机制，以在温和的操作条件下优化二氧化碳、一氧化碳和氧气的分离。为了实现这一目标，我们使用分子模拟和理想吸附溶液理论对可用沸石进行了基于拓扑结构和吸附性能的彻底筛选。FAU、BRE 和 MTW 被确定为这些分离过程的合适拓扑结构。FAU 可用于从一氧化碳和氧气中分离二氧化碳，而 BRE 或 MTW 可用于从氧气中分离一氧化碳。这些结果通过在室温下进行的变压吸附模拟得到了加强，该模拟将吸附柱与纯硅 FAU 沸石和 Si/Al 比为 3 的沸石 BRE 结合在一起。这些沸石还有一个额外的优点，即它们可商业化。
