Control of zeolite pore interior for chemoselective alkyne/olefin separations

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; Naijia Guan; Landong Li

doi:10.1126/science.aay8447

Control of zeolite pore interior for chemoselective alkyne/olefin separations

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, Naijia Guan, Landong Li

Research output: Contribution to journal › Article › peer-review

208 Scopus citations

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.

Original language	English
Pages (from-to)	1002-1006
Number of pages	5
Journal	Science
Volume	368
Issue number	6494
DOIs	https://doi.org/10.1126/science.aay8447
State	Published - May 29 2020

Funding

Supported by the National Natural Science Fund of China (21722303, 21421001, and 21688102), the Municipal Natural Science Fund of Tianjin (18JCJQJC47400 and 18JCZDJC37400), the 111 Project (B12015 and B18030), the U.K. Engineering and Physical Sciences Research Council (EP/P011632/1), and the University of Manchester and Newton Advanced Fellowship by the Royal Society (to W.S. and S.Yan.). Beamlines WISH and I11 were accessed through the STFC ISIS Facility and Diamond Light Source, respectively. INS experiments were conducted at the VISION beamline at ORNL's Spallation Neutron Source, which is supported by the Scientific User Facilities Division, Office of Basic Energy Sciences (BES), U.S. Department of Energy (DOE), under contract no. DE-AC0500OR22725 with UT Battelle, LLC. The computing resources were made available through the VirtuES and the ICEMAN projects, funded by the Laboratory Directed Research and Development program at ORNL

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title = "Control of zeolite pore interior for chemoselective alkyne/olefin separations",

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.",

author = "Yuchao Chai and Xue Han and Weiyao Li and Shanshan Liu and Sikai Yao and Chong Wang and Wei Shi and Ivan Da-Silva and Pascal Manuel and Yongqiang Cheng and Daemen, {Luke D.} and Ramirez-Cuesta, {Anibal J.} and Tang, {Chiu C.} and Ling Jiang and Sihai Yang and Naijia Guan and Naijia Guan and Landong Li",

year = "2020",

month = may,

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doi = "10.1126/science.aay8447",

language = "English",

volume = "368",

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journal = "Science",

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T1 - Control of zeolite pore interior for chemoselective alkyne/olefin separations

AU - Chai, Yuchao

AU - Han, Xue

AU - Li, Weiyao

AU - Liu, Shanshan

AU - Yao, Sikai

AU - Wang, Chong

AU - Shi, Wei

AU - Da-Silva, Ivan

AU - Manuel, Pascal

AU - Cheng, Yongqiang

AU - Daemen, Luke D.

AU - Ramirez-Cuesta, Anibal J.

AU - Tang, Chiu C.

AU - Jiang, Ling

AU - Yang, Sihai

AU - Guan, Naijia

AU - Li, Landong

PY - 2020/5/29

Y1 - 2020/5/29

N2 - 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.

AB - 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.

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DO - 10.1126/science.aay8447

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VL - 368

SP - 1002

EP - 1006

JO - Science

JF - Science

IS - 6494

ER -

Control of zeolite pore interior for chemoselective alkyne/olefin separations

Abstract

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