Abstract

Separation of C2H4 from C2H4/C2H2/C2H6 mixture with high working capacity is still a challenging task. Herein, we deliberately design a Th-metal-organic framework (MOF) for highly efficient separation of C2H4 from a binary C2H6/C2H4 and ternary C2H4/C2H2/C2H6 mixture. The synthesized MOF Azole-Th-1 shows a UiO-66-type structure with fcu topology built on a Th6 secondary building unit and a tetrazole-based linker. Such noticeable structure, is connected by a N,O-donor ligand with high chemical stability. At 100 kPa and 298 K Azole-Th-1 performs excellent separation of C2H4 (purity > 99.9%) from not only a binary C2H6/C2H4 (1:9, v/v) mixture but also a ternary mixture of C2H6/C2H2/C2H4 (9:1:90, v/v/v), and the corresponding working capacity can reach up to 1.13 and 1.34 mmol g−1, respectively. The separation mechanism, as unveiled by the density functional theory calculation, is due to a stronger van der Waals interaction between ethane and the MOF skeleton.

Highlights

  • Separation of C2H4 from C2H4/C2H2/C2H6 mixture with high working capacity is still a challenging task

  • Adsorptive separation by porous materials is an alternative technology, especially, some metal-organic frameworks (MOFs)[12,13,14,15,16,17,18,19,20,21] with high volume, designable pore characteristics, and countless structural possibilities, can be employed into the gas separation processes, the adsorption selectivity and capacity are higher than the results of conventional adsorbents[22,23,24] such as zeolites and carbon-based, especially the adsorption and separation for C2H6/C2H48,22,25–39

  • We reported a Th-azole framework (Azole-Th-1) by introducing an previously unreported ligand TBA showing a preferential adsorption of ethane over ethylene

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Summary

Introduction

Separation of C2H4 from C2H4/C2H2/C2H6 mixture with high working capacity is still a challenging task. Lu and co-workers[49] report that they use TJT-100 to obtain the selective adsorption of ethane and acetylene over ethylene from a ternary mixture of C2H2/C2H6/C2H4 (0.5:0.5:99, v/v/v) and achieve a C2H4 purity greater than 99.9% (working capacity of 0.69 mmol g−1) by a single-breakthrough operation. Zaworoko et al.[38] use a synergistic sorbent separation method for the one-step production of polymer-grade C2H4 from ternary (C2H2/C2H6/C2H4, working capacity of 0.32 mmol g−1) or quaternary (CO2/C2H2/C2H6/C2H4) gas mixtures with a series of physisorbents. In this regard, constructing MOFs with high working capacity is still highly desirable from the viewpoint of practical application

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