Green Synthesis of MOF-801(Zr/Ce/Hf) for CO<sub>2</sub>/N<sub>2</sub> and CO<sub>2</sub>/CH<sub>4</sub> Separation

Chen-Ning Li (15452491), Shi-Ming Wang (1616362), Zhi-Peng Tao (15452494), Lin Liu (74495), Wei-Guo Xu (1793728), Xue-Jun Gu (15452497), Zheng-Bo Han (1616368)
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Abstract

The\npurification of natural gas and the removal of carbon dioxide\nfrom flue gases are crucial to economize precious resources and effectively\nrelieve a series of environmental problems caused by global warming.\nMetal–organic framework (MOF) materials have demonstrated remarkable\nperformance and benefits in the area of gas separation; however, obtaining\nmaterials with high gas capacity and selectivity simultaneously remains\ndifficult. In addition, harsh synthesis conditions and solvent toxicity\nhave been restricted in large-scale production and industrial application.\nTherefore, MOF-801(Zr/Ce/Hf) was created based on the green synthesis\nof the MOF-801 construction unit by altering the kinds of metal salts,\nand the impact of three metal nodes on the performance of gas adsorption\nand separation was demonstrated by contrasting the three MOFs. The\nresults showed that MOF-801(Ce) has the best CO<sub>2</sub> adsorption\ncapacity (3.3 mmol/g at 298 K), which also was demonstrated with in\nsitu diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS)\nresults, CO<sub>2</sub>/CH<sub>4</sub> (ideal adsorbed solution theory\n(IAST) = 13.28 at 298 K, 1 bar, CO<sub>2</sub>/CH<sub>4</sub> = 1:1,\nv/v), and the separation performance of CO<sub>2</sub>/N<sub>2</sub> (IAST = 57.46 at 298 K, 1 bar, CO<sub>2</sub>/N<sub>2</sub> = 1:1,\nv/v) among the group. Green synthesis of MOF-801(Zr/Ce/Hf) is an ideal\ncandidate for flue gas separation and methane purification because\nof its high regeneration capacity and strong cyclic stability.
CO<sub>2</sub>/N<sub>2</sub>;和CO<;sub>2</sub>/CH<sub>4</sub>;分离MOF-801(Zr/Ce/Hf)的绿色合成
天然气的净化和烟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引起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显著的性能和优势;然而,同时获得具有高气体容量和选择性的材料仍然是困难的。此外,合成条件苛刻,溶剂毒性大,限制了其大规模生产和工业应用。因此,通过改变金属盐的种类,在绿色合成的基础上制备了MOF-801(Zr/Ce/Hf),并通过对三种mof的对比,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<;sub>2</sub>/ sub>;吸附容量(298 K时为3.3 mmol/g),这一结果也得到了原位弥漫反射红外傅里叶变换光谱(DRIFTS)结果的证明,CO<sub>2</sub>/CH<sub>4</sub>(理想吸附溶液理论\n(IAST) = 13.28, 298 K, 1 bar时,CO<sub>2</sub>/CH<sub>4</sub> = 1:1,\nv/v);CO<sub>2</sub>/N<sub>2</ sub< (IAST = 57.46, 298 K, 1 bar, CO<sub>2</ N<sub>2</sub> = 1:1,\nv/v)组间分离性能。绿色合成MOF-801(Zr/Ce/Hf)具有较高的再生能力和较强的循环稳定性,是烟气分离和甲烷净化的理想候选材料。
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