Control of zeolite pore interior for chemoselective alkyne/olefin separations

DOI: 10.1126/science.aay8447

Authors: Yuchao Chai (Nankai University) , Xue Han (The University of Manchester) , Weiyao Li (The University of Manchester) , Shanshan Liu (Nankai University) , Sikai Yao (Nankai University) , Chong Wang (Dalian Institute of Chemical Physics, Chinese Academy of Sciences) , Wei Shi (Nankai University) , Ivan Da Silva (ISIS Facility) , Pascal Manuel (ISIS Facility) , Yongqiang Cheng (Oak Ridge National Laboratory (ORNL)) , Luke D. Daemen (Oak Ridge National Laboratory (ORNL)) , Anibal J. Ramirez-cuesta (Oak Ridge National Laboratory (ORNL)) , Chiu C. Tang (Diamond Light Source) , Ling Jiang (Dalian Institute of Chemical Physics, Chinese Academy of Sciences) , Sihai Yang (The University of Manchester) , Naijia Guan (Nankai University;) , Landong Li (Nankai University)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Science , VOL 368 , PAGES 1002 - 1006

State: Published (Approved)
Published: May 2020
Diamond Proposal Number(s): 23483

Abstract: The efficient removal of alkyne impurities for the production of polymer-grade lower olefins remains an important and challenging goal for many industries. We report a strategy to control the pore interior of faujasite (FAU) zeolites by the confinement of isolated open nickel(II) sites in their six-membered rings. Under ambient conditions, Ni@FAU showed remarkable adsorption of alkynes and efficient separations of acetylene/ethylene, propyne/propylene, and butyne/1,3-butadiene mixtures, with unprecedented dynamic separation selectivities of 100, 92, and 83, respectively. In situ neutron diffraction and inelastic neutron scattering revealed that confined nickel(II) sites enabled chemoselective and reversible binding to acetylene through the formation of metastable [Ni(II)(C2H2)3] complexes. Control of the chemistry of pore interiors of easily scalable zeolites has unlocked their potential in challenging industrial separations.

Subject Areas: Chemistry


Instruments: I11-High Resolution Powder Diffraction

Documents:
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