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Research Article

Selective adsorption of liquid long-chain α-olefin/paraffin on Mg-MOF-74: Adsorption behavior and interaction mechanism

Ruihan Yang1Shafqat Ullah1Xiao Chen2Junxiang Ma3Yuan Gao3Yujun Wang1( )Guangsheng Luo1
State Key Lab of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
Lu’an Chemical Group Co., Ltd., Changzhi 046299, China
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Graphical Abstract

The selective adsorption performance, adsorption sites, and different interaction contributions of liquid longchain α-olefin/paraffin on Mg-metal–organic framework (MOF)-74 are investigated using a combination of batch adsorption experiments and molecular simulation techniques, which provides a general method and guidance for liquid adsorption separation and host-guest interactions during the adsorption or catalytic process of nanoporous materials.

Abstract

The liquid products of Fischer–Tropsch synthesis with a high content of linear α-olefins can act as valuable raw materials for increasing high added-value α-olefin production if the challenging separation of long-chain α-olefin/paraffin is achieved. Adsorption separation is an efficient alternative to energy-intensive distillation. Herein, the selective adsorption behavior and interaction mechanism of liquid α-olefin/paraffin on Mg metal–organic framework (MOF)-74 were investigated using a combination of batch adsorption experiments and molecular simulation techniques. Mg-MOF-74 exhibited 301 and 333 mg/g olefin adsorption capacities for C6 and C8 linear α-olefins in binary olefin/paraffin mixtures, respectively, and was still unsaturated at high olefin concentrations. The adsorption isotherms were analyzed and compared with the simulated results by configurational-bias grand canonical Monte Carlo (CB-GCMC) simulation. The visualized adsorption sites by CB-GCMC simulation indicated that all adsorbates were arranged in hexagonal shapes and preferentially adsorbed by the vertex of the hexagon, where the metal node magnesium is located. The adsorption energies were −1.456 and −0.378 eV for C8 linear α-olefin and paraffin, respectively, calculated by density functional theory simulation based on the visualized adsorption sites. The charge transfer was analyzed, and the contributions of different kinds of interactions to the overall adsorption energy were quantified by principle orbital interaction analysis to further reveal the difference in adsorption energy between α-olefin/paraffin and Mg-MOF-74. This work also provides a general means to investigate the liquid adsorption performance and host–guest interactions in the adsorption or catalytic processes of nanoporous materials.

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Nano Research
Pages 1595-1605
Cite this article:
Yang R, Ullah S, Chen X, et al. Selective adsorption of liquid long-chain α-olefin/paraffin on Mg-MOF-74: Adsorption behavior and interaction mechanism. Nano Research, 2023, 16(1): 1595-1605. https://doi.org/10.1007/s12274-022-4796-2
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Received: 07 April 2022
Revised: 14 July 2022
Accepted: 20 July 2022
Published: 02 September 2022
© Tsinghua University Press 2022
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