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Control of zeolite pore interior for chemoselective alkyne/olefin separations
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:
1002.full.pdf