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A Trifluoromethyl-Functionalized Ni-MOF with Fluorinated Pore Surface for One-Step Purification of Polymer-Grade C2H4
Jun Chen1,2, Tao Cui3, Bingjie Ruan3
1Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, Nanjing Drum Tower Hospital, College of Chemistry and Materials Science, Nanjing Normal University, Nanjing210023, China.
Abstract:
Efficient purification of polymer-grade ethylene (C2H4) from methanol-to-olefins (MTO) products remains challenging because of the similar physicochemical properties of light hydrocarbons. Herein, we report a fluorinated metal-organic framework, CF3-Ni, featuring uniformly distributed trifluoromethyl (-CF3) groups that construct a fluorine-rich polar pore environment for selective hydrocarbon recognition. CF3-Ni exhibits preferential adsorption toward C3 hydrocarbons, with an affinity sequence of C3H6 > C3H8 > C2H4. At 298 K and 1 bar, it shows a C3H6/C2H4 IAST selectivity of 9.3 and a moderate C3H6 adsorption enthalpy of 38.4 kJ mol-1, enabling strong yet reversible host-guest interactions. Breakthrough experiments demonstrate efficient separation of C3H6/C2H4 mixtures over a wide range of feed compositions, affording polymer-grade C2H4 (>99.95%) with a maximum productivity of 7.4 mol kg-1 and simultaneous recovery of high-purity C3H6. Notably, one-step purification of polymer-grade C2H4 is achieved from a ternary C3H6/C3H8/C2H4 mixture, even under humid and elevated-pressure conditions. DFT calculations and in situ FT-IR spectroscopy reveal that C-H···F interactions contribute to the preferential binding of C3H6. This work demonstrates fluorinated pore chemistry as an effective strategy for practical olefin purification.
