Control of zeolite pore interior for chemoselective alkyne/olefin separations



论文题目:Control of zeolite pore interior for chemoselective alkyne/olefin separations

论文作者:Yuchao Chai*, Xue Han*, Weiyao Li, Shanshan Liu, Sikai Yao, Chong Wang, Wei Shi, Ivan da-Silva, Pascal Manuel, Yongqiang Cheng, Luke D. Daemen, Anibal J. Ramirez-Cuesta, Chiu C. Tang, Ling Jiang, Sihai Yang†,Naijia Guan, Landong Li†

发表期刊:Science, 2020, 368(6494), 1002-1006     


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.