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Carbohydrate-Mediated Purification of Petrochemicals

Lookup NU author(s): James Holcroft, Dr Jon Bell, Emeritus Professor Mark ThomasORCiD

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This work is licensed under a Creative Commons Attribution-NonCommercial 4.0 International License (CC BY-NC 4.0).


Abstract

Metal-organic frameworks (MOFs) are known to facilitate energy-efficient separations of important industrial chemical feedstocks. Here, we report how a class of green MOFs – namely CD-MOFs – exhibits high shape-selectivity towards aromatic hydrocarbons. CDMOFs, which consist of an extended porous network of γ-cyclodextrins (γ-CDs) and alkali metal cations, can separate a wide range of benzenoid compounds as a result of their relative orientation and packing within the transverse channels, formed from linking (γ-CD)6 body-centered cuboids in three dimensions. Adsorption isotherms and liquid-phase chromatographic measurements indicate a retention order of ortho- > meta- > para-xylene. The persistence of this regioselectivity is also observed during the liquid-phase chromatography of the ethyltoluene and cymene regioisomers. In addition, molecular shape-sorting within CD-MOFs facilitates the separation of the industrially relevant BTEX (Benzene, Toluene, Ethylbenzene and the Xylene isomers) mixture. The high resolution and large separation factors exhibited by CD-MOFs for benzene and these alkylaromatics provide an efficient, reliable and green alternative to current isolation protocols. Furthermore, the isolation of the regioisomers of (i) ethyltoluene and (ii) cymene, together with the purification of (iii) cumene from its major impurities (benzene, n-propylbenzene and diisopropylbenzene), highlight the specificity of the shape-selectivity exhibited by CD-MOFs. Grand canonical Monte Carlo (GCMC) simulations and single component static vapor adsorption isotherms and kinetics reveal the origin of the shape-selectivity and provide insight into the capability of CD-MOFs to serve as versatile separation platforms derived from renewable sources.


Publication metadata

Author(s): Holcroft JM, Hartlieb KJ, Moghadam PZ, Bell JG, Barin G, Ferris DP, Bloch ED, Algradah MM, Nassar MS, Botros YY, Thomas KM, Long JR, Snurr RQ, Stoddart JF

Publication type: Article

Publication status: Published

Journal: Journal of the American Chemical Society

Year: 2015

Volume: 137

Issue: 17

Pages: 5706-5719

Print publication date: 06/05/2015

Online publication date: 25/03/2015

Acceptance date: 25/03/2015

Date deposited: 16/04/2015

ISSN (print): 0002-7863

ISSN (electronic): 1520-5126

Publisher: American Chemical Society

URL: http://dx.doi.org/10.1021/ja511878b

DOI: 10.1021/ja511878b


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Funding

Funder referenceFunder name
Miller Institute for Basic Research in Science, University of California, Berkeley
34-947Joint Center of Excellence in Integrated Nano-Systems (JCIN Project) at King Abdulaziz City for Science and Technology (KACST)
EP/K005499/1ESPRC
DE-SC0001015Center for Gas Separations Relevant to Clean Energy Technologies, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences
P20261Northwestern University
W911NF-12-1-0130Army Research Office

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