Control of zeolite pore interior for chemoselective alkyne/olefin separations

被引：278

作者：

Chai, Yuchao ^{[1
,2
]}

Han, Xue ^{[3
]}

Li, Weiyao ^{[3
]}

Liu, Shanshan ^{[1
,2
]}

Yao, Sikai ^{[1
,2
]}

Wang, Chong ^{[4
]}

Shi, Wei ^{[5
]}

da-Silva, Ivan ^{[6
]}

Manuel, Pascal ^{[6
]}

Cheng, Yongqiang ^{[7
]}

Daemen, Luke D. ^{[7
]}

Ramirez-Cuesta, Anibal J. ^{[7
]}

Tang, Chiu C. ^{[8
]}

Jiang, Ling ^{[4
]}

Yang, Sihai ^{[3
]}

Guan, Naijia ^{[1
,2
,5
]}

Li, Landong ^{[1
,2
,5
]}

机构：

[1] Nankai Univ, Sch Mat Sci & Engn, Tianjin 300350, Peoples R China

[2] Nankai Univ, Natl Inst Adv Mat, Tianjin 300350, Peoples R China

[3] Univ Manchester, Dept Chem, Manchester M13 9PL, Lancs, England

[4] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China

[5] Nankai Univ, Key Lab Adv Energy Mat Chem, Minist Educ, Tianjin 300071, Peoples R China

[6] Rutherford Appleton Lab, ISIS Facil, Sci & Technol Facil Council STFC, Chilton OX11 0QX, Oxon, England

[7] Oak Ridge Natl Lab ORNL, Neutron Scattering Div, Neutron Sci Directorate, Oak Ridge, TN 37831 USA

[8] Diamond Light Source, Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England

来源：

SCIENCE | 2020年 / 368卷 / 6494期

基金：

英国工程与自然科学研究理事会;

关键词：

METAL-ORGANIC FRAMEWORK; EFFICIENT REMOVAL; ACETYLENE; NICKEL; ADSORPTION; ETHYLENE; THERMODYNAMICS; DEHYDRATION; PALLADIUM; CATALYSTS;

D O I：

10.1126/science.aay8447

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

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.

引用

页码：1002 / +

页数：77

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