Direct Ethylene Purification from Cracking Gas via a Metal–Organic Framework Through Pore Geometry Fitting

IF 10.1 1区工程技术 Q1 ENGINEERING, MULTIDISCIPLINARY Engineering Pub Date : 2024-10-01 DOI:10.1016/j.eng.2024.01.024

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Abstract

The direct one-step separation of polymer-grade C₂H₄ from complex light hydrocarbon mixtures has high industrial significance but is very challenging. Herein, an ethylene-adsorption-weakening strategy is applied for precise regulation of the pore geometry of four tailor-made metal–organic frameworks (MOFs) with pillar-layered structures, dubbed TYUT-10/11/12/13. Based on its pore geometry design and functional group regulation, TYUT-12 exhibits exceptional selective adsorption selectivity toward C₃H₈, C₃H₆, C₂H₆, C₂H₂, and CO₂ over C₂H₄; its C₂H₆/C₂H₄ adsorption selectivity reaches 4.56, surpassing the record value of 4.4 by Fe₂(O₂)(dobdc) (dobdc⁴⁻ = 2,5-dioxido-1,4-benzenedicarboxylate). The weak π–π stacking binding affinity toward C₂H₄ in TYUT-12 is clearly demonstrated through a combination of neutron powder diffraction measurements and theoretical calculations. Breakthrough experiments demonstrate that C₂H₄ can be directly obtained from binary, ternary, quaternary, and six-component light hydrocarbon mixtures with over 99.95% purity.

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通过孔几何拟合金属有机框架从裂解气中直接提纯乙烯

从复杂的轻烃混合物中一步直接分离出聚合物级 C2H4 具有重要的工业意义，但却非常具有挑战性。本文采用乙烯吸附弱化策略精确调节了四种具有柱层结构的定制金属有机框架（MOFs）（命名为 TYUT-10/11/12/13）的孔几何形状。基于其孔隙几何设计和官能团调节，TYUT-12 对 C3H8、C3H6、C2H6、C2H2 和 CO2 的吸附选择性超过了 C2H4；其对 C2H6/C2H4 的吸附选择性达到了 4.56，超过了 Fe2(O2)(dobdc)（dobdc4- = 2,5-二氧代-1,4-苯二甲酸酯）的 4.4 记录值。中子粉末衍射测量和理论计算相结合，清楚地证明了 TYUT-12 中 C2H4 的弱π-π 堆积结合亲和力。突破性实验证明，可以直接从二元、三元、四元和六元轻烃混合物中获得 C2H4，纯度超过 99.95%。

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来源期刊

Engineering Environmental Science-Environmental Engineering

自引率

1.60%

发文量

335

审稿时长

35 days

期刊介绍： Engineering, an international open-access journal initiated by the Chinese Academy of Engineering (CAE) in 2015, serves as a distinguished platform for disseminating cutting-edge advancements in engineering R&D, sharing major research outputs, and highlighting key achievements worldwide. The journal's objectives encompass reporting progress in engineering science, fostering discussions on hot topics, addressing areas of interest, challenges, and prospects in engineering development, while considering human and environmental well-being and ethics in engineering. It aims to inspire breakthroughs and innovations with profound economic and social significance, propelling them to advanced international standards and transforming them into a new productive force. Ultimately, this endeavor seeks to bring about positive changes globally, benefit humanity, and shape a new future.