Fu Jia, Wu Jianzhong, Custelcean Radu, Jiang De-En
Department of Chemical and Environmental Engineering, University of California, Riverside, CA 92521, United States.
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, United States.
J Colloid Interface Sci. 2015 Jan 15;438:191-195. doi: 10.1016/j.jcis.2014.09.079. Epub 2014 Oct 7.
Recently synthesized porous aromatic frameworks (PAFs) exhibit extremely high surface areas and exceptional thermal and hydrothermal stabilities. Using computer-aided design, we propose new PAFs, designated as NPAFs, by introducing nitrogen-containing groups to the biphenyl unit and predict their CO2 adsorption capacities with grand canonical Monte Carlo (GCMC) simulations. Among various NPAFs considered, one with imidazole groups shows the highest adsorption capacity for CO2 (11.5 wt% at 1 bar and 298 K), in comparison with 5 wt% for the parent PAF (PAF-1) at the same condition. At higher pressures (around 10 bar), however, another NPAF with pyridinic N groups performs much better than the rest due to its greater pore volume in addition to the N functionality. This study suggests that adding N functionality to the organic linkers is a promising way to increase CO2 adsorption capacity of PAFs at ambient condition.
最近合成的多孔芳香框架材料（PAFs）具有极高的比表面积以及出色的热稳定性和水热稳定性。通过计算机辅助设计，我们通过在联苯单元中引入含氮基团，提出了一种新的PAFs，命名为NPAFs，并通过巨正则蒙特卡罗（GCMC）模拟预测了它们对CO₂的吸附容量。在考虑的各种NPAFs中，带有咪唑基团的一种对CO₂的吸附容量最高（在1 bar和298 K条件下为11.5 wt%），相比之下，在相同条件下母体PAF（PAF-1）的吸附容量为5 wt%。然而，在更高压力（约10 bar）下，另一种带有吡啶型N基团的NPAF表现比其他材料好得多，这是因为除了N官能团外，它还具有更大的孔体积。这项研究表明，在有机连接体中添加N官能团是在环境条件下提高PAFs对CO₂吸附容量的一种有前途的方法。
