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Carbon nanotube supported oriented metal organic framework membrane for effective ethylene/ethane separation.

ABSTRACT: Zeolitic imidazolate framework 8 (ZIF-8) is effective for C₃H₆/C₃H₈ separation because of the "sieving effect" of a six-membered (6-M) window. Here, we demonstrate that ZIF-8 is a versatile material that could effectively separate C₂H₄ from C₂H₆ via its 4-M window along the <100> direction. We established a facile and environmentally friendly carbon nanotube (CNT)-induced oriented membrane (CNT-OM) approach to fabricate a {100}-oriented ZIF-8 membrane (100-M). In this approach, 2-methyimidazole was anchored onto the CNT surface followed by 3-hour in situ growth in aqueous solution at room temperature. The obtained 100-M, whose 4-M window is aligned along the transport pathway, showed ~3 times higher C₂H₄/C₂H₆ selectivity than a randomly oriented membrane. Thus, this work demonstrates that the membrane orientation plays an important role in tuning selectivity toward different gas pairs. Furthermore, 100-M exhibited excellent mechanical stability that could sustain the separation performance after bending at a curvature of ~109 m^-1.

SUBMITTER: Wei R

PROVIDER: S-EPMC8849294 | biostudies-literature | 2022 Feb

REPOSITORIES: biostudies-literature

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Carbon nanotube supported oriented metal organic framework membrane for effective ethylene/ethane separation.

Wei Ruicong R Liu Xiaowei X Zhou Zongyao Z Chen Cailing C Yuan Youyou Y Li Zhen Z Li Xiang X Dong Xinglong X Lu Dongwei D Han Yu Y Lai Zhiping Z

Science advances 20220216 7

Zeolitic imidazolate framework 8 (ZIF-8) is effective for C3H6/C3H8 separation because of the "sieving effect" of a six-membered (6-M) window. Here, we demonstrate that ZIF-8 is a versatile material that could effectively separate C2H4 from C2H6 via its 4-M window along the <100> direction. We established a facile and environmentally friendly carbon nanotube (CNT)-induced oriented membrane (CNT-OM) approach t ...[more]

PMID: 35171662

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Project description:Ethylene dimerization is an efficient industrial chemical process to produce 1-butene, with demanding selectivity and activity requirements on new catalytic systems. Herein, a series of monodentate phosphinoamine-nickel complexes immobilized on UiO-66 are described for ethylene dimerization. These catalysts display extensive molecular tunability of the ligand similar to organometallic catalysis, while maintaining the high stability attributed to the metal-organic framework (MOF) scaffold. The highly flexible postsynthetic modification method enables this study to prepare MOFs functionalized with five different substituted phosphines and 3 N-containing ligands and identify the optimal catalyst UiO-66-L5-NiCl2 with isopropyl substituted nickel mono-phosphinoamine complex. This catalyst shows a remarkable activity and selectivity with a TOF of 29 000 (molethyl/molNi/h) and 99% selectivity for 1-butene under ethylene pressure of 15 bar. The catalyst is also applicable for continuous production in the packed column micro-reactor with a TON of 72 000 (molethyl/molNi). The mechanistic insight for the ethylene oligomerization has been examined by density functional theory (DFT) calculations. The calculated energy profiles for homogeneous complexes and truncated MOF models reveal varying rate-determining step as β-hydrogen elimination and migratory insertion, respectively. The activation barrier of UiO-66-L5-NiCl2 is lower than other systems, possibly due to the restriction effect caused by clusters and ligands. A comprehensive analysis of the structural parameters of catalysts shows that the cone angle as steric descriptor and butene desorption energy as thermodynamic descriptor can be applied to estimate the reactivity turnover frequency (TOF) with the optimum for UiO-66-L5-NiCl2. This work represents the systematic optimization of ligand effect through combination of experimental and theoretical data and presents a proof-of-concept for ethylene dimerization catalyst through simple heterogenization of organometallic catalyst on MOF.

Dataset Information

Carbon nanotube supported oriented metal organic framework membrane for effective ethylene/ethane separation.

Publications

Carbon nanotube supported oriented metal organic framework membrane for effective ethylene/ethane separation.

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