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Fine-tuning of pore-space-partitioned metal-organic frameworks for efficient C2H2/C2H4 and C2H2/CO2 separation
Chinese Chemical Letters ( IF 9.4 ) Pub Date : 2022-03-07 , DOI: 10.1016/j.cclet.2022.03.019
Xiaobing Mu 1 , Yingying Xue 1 , Mancheng Hu 1 , Peng Zhang 1 , Ying Wang 1 , Haipeng Li 1 , Shuni Li 1 , Quanguo Zhai 1
Affiliation  

Acetylene (C2H2) and ethylene (C2H4) both are important chemical raw materials and energy fuel gases. But the effective removement of trace C2H2 from C2H4 and the purification of C2H2 from carbon dioxide (CO2) are particularly challenging in the petrochemical industry. As a class of porous physical adsorbent, metal-organic frameworks (MOFs) have exhibited great success in separation and purification of light hydrocarbon gas. Herein, we rationally designed four novel MOFs by the strategy of pore space partition (PSP) via introducing triangular tri(pyridin-4-yl)-amine (TPA) into the 1D hexagonal channels of acs-type parent skeleton. By modulating the functional groups of linear dicarboxylate linkers for the parent skeleton, a series of iso-reticular PSP-MOFs (SNNU-278−281) were successfully obtained. The synergistic effects of suitable pore size and Lewis basic functional groups make these MOFs ideal C2H2 adsorbents. The gas adsorption experimental results show that all MOFs have excellent C2H2 uptakes. Specially, SNNU-278 demonstrates a high C2H2 uptake of 149.7 cm3/g at 273 K and 1 atm. Meanwhile, SNNU-278−281 MOFs also show extremely great C2H2 separation from CO2 and C2H4. The optimized SNNU-281 with high-density hydroxy groups exhibits extraordinary C2H2/CO2 and C2H2/C2H4 dynamic breakthrough interval times up to 31 min/g and 17 min/g under 298 K and 1 bar.



中文翻译:

微调孔隙空间分区金属有机框架,以实现高效的 C2H2/C2H4 和 C2H2/CO2 分离

乙炔(C 2 H 2)和乙烯(C 2 H 4)都是重要的化工原料和能源燃料气体。但是,从 C 2 H 4中有效去除痕量 C 2 H 2以及从二氧化碳 (CO 2 ) 中纯化 C 2 H 2在石化工业中尤其具有挑战性。作为一类多孔物理吸附剂,金属有机骨架(MOFs)在轻烃气体的分离和纯化方面取得了巨大的成功。在此,我们通过孔隙空间分配(PSP)的策略合理地设计了四种新型MOFs将三角形三(吡啶-4-基)-胺(TPA)引入acs型母体骨架的一维六边形通道。通过调节母体骨架的线性二羧酸酯接头的官能团,成功获得了一系列等网状 PSP-MOFs (SNNU-278-281)。合适的孔径和路易斯碱性官能团的协同作用使这些MOFs成为理想的C 2 H 2吸附剂。气体吸附实验结果表明,所有MOFs都具有优异的C 2 H 2吸收率。特别是,SNNU-278在 273 K 和 1 个大气压下表现出 149.7 cm 3 /g 的高 C 2 H 2吸收。同时,SNNU-278−281 MOFs 也表现出极好的 C 2 H2从CO 2和C 2 H 4中分离。具有高密度羟基优化SNNU - 281在298 K1 _酒吧。

更新日期:2022-03-07
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