College of Chemistry, Liaoning University. Shenyang 110036, P. R. China.
Light Industry College, Liaoning University, Shenyang 110036, P. R. China.
Inorg Chem. 2023 May 22;62(20):7853-7860. doi: 10.1021/acs.inorgchem.3c00560. Epub 2023 May 11.
The purification of natural gas and the removal of carbon dioxide from flue gases are crucial to economize precious resources and effectively relieve a series of environmental problems caused by global warming. Metal-organic framework (MOF) materials have demonstrated remarkable performance and benefits in the area of gas separation; however, obtaining materials with high gas capacity and selectivity simultaneously remains difficult. In addition, harsh synthesis conditions and solvent toxicity have been restricted in large-scale production and industrial application. Therefore, MOF-801(Zr/Ce/Hf) was created based on the green synthesis of the MOF-801 construction unit by altering the kinds of metal salts, and the impact of three metal nodes on the performance of gas adsorption and separation was demonstrated by contrasting the three MOFs. The results showed that MOF-801(Ce) has the best CO adsorption capacity (3.3 mmol/g at 298 K), which also was demonstrated with in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results, CO/CH (ideal adsorbed solution theory (IAST) = 13.28 at 298 K, 1 bar, CO/CH = 1:1, v/v), and the separation performance of CO/N (IAST = 57.46 at 298 K, 1 bar, CO/N = 1:1, v/v) among the group. Green synthesis of MOF-801(Zr/Ce/Hf) is an ideal candidate for flue gas separation and methane purification because of its high regeneration capacity and strong cyclic stability.
天然气的净化和烟道气中二氧化碳的去除对于节约宝贵资源和有效缓解全球变暖带来的一系列环境问题至关重要。金属有机骨架(MOF)材料在气体分离领域表现出了优异的性能和优势;然而,同时获得高气体容量和选择性的材料仍然具有挑战性。此外,苛刻的合成条件和溶剂毒性限制了其在大规模生产和工业应用中的应用。因此,通过改变金属盐的种类,基于 MOF-801 结构单元的绿色合成,制备了 MOF-801(Zr/Ce/Hf),并通过对比三种 MOF 证明了三种金属节点对气体吸附和分离性能的影响。结果表明,MOF-801(Ce)具有最佳的 CO 吸附容量(298 K 时为 3.3 mmol/g),这也通过原位漫反射红外傅里叶变换光谱(DRIFTS)结果、CO/CH(理想吸附溶液理论(IAST)= 13.28 得到了证明,在 298 K、1 bar 下,CO/CH = 1:1,v/v)和 CO/N 的分离性能(IAST = 57.46,在 298 K、1 bar 下,CO/N = 1:1,v/v)。由于其高再生能力和强循环稳定性,MOF-801(Zr/Ce/Hf)的绿色合成是烟道气分离和甲烷净化的理想候选材料。