Extraordinary Separation of Acetylene-Containing Mixtures with Microporous Metal-Organic Frameworks with Open O Donor Sites and Tunable Robustness through Control of the Helical Chain Secondary Building Units

Handle URI:
http://hdl.handle.net/10754/621664
Title:
Extraordinary Separation of Acetylene-Containing Mixtures with Microporous Metal-Organic Frameworks with Open O Donor Sites and Tunable Robustness through Control of the Helical Chain Secondary Building Units
Authors:
Yao, Zizhu; Zhang, Zhangjing; Liu, Lizhen; Li, Ziyin; Zhou, Wei; Zhao, Yunfeng; Han, Yu ( 0000-0003-1462-1118 ) ; Chen, Banglin; Krishna, Rajamani; Xiang, Shengchang ( 0000-0001-6016-2587 )
Abstract:
Acetylene separation is a very important but challenging industrial separation task. Here, through the solvothermal reaction of CuI and 5-triazole isophthalic acid in different solvents, two metal-organic frameworks (MOFs, FJU-21 and FJU-22) with open O donor sites and controllable robustness have been obtained for acetylene separation. They contain the same paddle-wheel {Cu2(COO2)4} nodes and metal-ligand connection modes, but with different helical chains as secondary building units (SBUs), leading to different structural robustness for the MOFs. FJU-21 and FJU-22 are the first examples in which the MOFs' robustness is controlled by adjusting the helical chain SBUs. Good robustness gives the activated FJU-22 a, which has higher surface area and gas uptakes than the flexible FJU-21 a. Importantly, FJU-22 a shows extraordinary separation of acetylene mixtures under ambient conditions. The separation capacity of FJU-22 a for 50:50 C2H2/CO2 mixtures is about twice that of the high-capacity HOF-3, and its actual separation selectivity for C2H2/C2H4 mixtures containing 1 % acetylene is the highest among reported porous materials. Based on first-principles calculations, the extraordinary separation performance of C2H2 for FJU-22 a was attributed to hydrogen-bonding interactions between the C2H2 molecules with the open O donors on the wall, which provide better recognition ability for C2H2 than other functional sites, including open metal sites and amino groups. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division
Citation:
Yao Z, Zhang Z, Liu L, Li Z, Zhou W, et al. (2016) Extraordinary Separation of Acetylene-Containing Mixtures with Microporous Metal-Organic Frameworks with Open O Donor Sites and Tunable Robustness through Control of the Helical Chain Secondary Building Units. Chem Eur J 22: 5676–5683. Available: http://dx.doi.org/10.1002/chem.201505107.
Publisher:
Wiley-Blackwell
Journal:
Chemistry - A European Journal
Issue Date:
2-Mar-2016
DOI:
10.1002/chem.201505107
Type:
Article
ISSN:
0947-6539
Sponsors:
This work was financially supported by the National Natural Science Foundation of China (21207018, 21273033, 21203024, and 21573042) and the Fujian Science and Technology Department (2014J06003 and 2014H6007). S.X. gratefully acknowledges the support of the Recruitment Program of Global Young Experts, Program for New Century Excellent Talents in University (NCET-10-0108), and the Award 'MinJiang Scholar Program' in Fujian Province.
Is Supplemented By:
Yao, Z., Zhang, Z., Liu, L., Li, Z., Zhou, W., Zhao, Y., … Xiang, S. (2016). CCDC 1421052: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1jpqdb; DOI:10.5517/ccdc.csd.cc1jpqdb; HANDLE:http://hdl.handle.net/10754/624521; Yao, Z., Zhang, Z., Liu, L., Li, Z., Zhou, W., Zhao, Y., … Xiang, S. (2016). CCDC 1421054: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1jpqgd; DOI:10.5517/ccdc.csd.cc1jpqgd; HANDLE:http://hdl.handle.net/10754/624522
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorYao, Zizhuen
dc.contributor.authorZhang, Zhangjingen
dc.contributor.authorLiu, Lizhenen
dc.contributor.authorLi, Ziyinen
dc.contributor.authorZhou, Weien
dc.contributor.authorZhao, Yunfengen
dc.contributor.authorHan, Yuen
dc.contributor.authorChen, Banglinen
dc.contributor.authorKrishna, Rajamanien
dc.contributor.authorXiang, Shengchangen
dc.date.accessioned2016-11-03T13:22:13Z-
dc.date.available2016-11-03T13:22:13Z-
dc.date.issued2016-03-02en
dc.identifier.citationYao Z, Zhang Z, Liu L, Li Z, Zhou W, et al. (2016) Extraordinary Separation of Acetylene-Containing Mixtures with Microporous Metal-Organic Frameworks with Open O Donor Sites and Tunable Robustness through Control of the Helical Chain Secondary Building Units. Chem Eur J 22: 5676–5683. Available: http://dx.doi.org/10.1002/chem.201505107.en
dc.identifier.issn0947-6539en
dc.identifier.doi10.1002/chem.201505107en
dc.identifier.urihttp://hdl.handle.net/10754/621664-
dc.description.abstractAcetylene separation is a very important but challenging industrial separation task. Here, through the solvothermal reaction of CuI and 5-triazole isophthalic acid in different solvents, two metal-organic frameworks (MOFs, FJU-21 and FJU-22) with open O donor sites and controllable robustness have been obtained for acetylene separation. They contain the same paddle-wheel {Cu2(COO2)4} nodes and metal-ligand connection modes, but with different helical chains as secondary building units (SBUs), leading to different structural robustness for the MOFs. FJU-21 and FJU-22 are the first examples in which the MOFs' robustness is controlled by adjusting the helical chain SBUs. Good robustness gives the activated FJU-22 a, which has higher surface area and gas uptakes than the flexible FJU-21 a. Importantly, FJU-22 a shows extraordinary separation of acetylene mixtures under ambient conditions. The separation capacity of FJU-22 a for 50:50 C2H2/CO2 mixtures is about twice that of the high-capacity HOF-3, and its actual separation selectivity for C2H2/C2H4 mixtures containing 1 % acetylene is the highest among reported porous materials. Based on first-principles calculations, the extraordinary separation performance of C2H2 for FJU-22 a was attributed to hydrogen-bonding interactions between the C2H2 molecules with the open O donors on the wall, which provide better recognition ability for C2H2 than other functional sites, including open metal sites and amino groups. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.en
dc.description.sponsorshipThis work was financially supported by the National Natural Science Foundation of China (21207018, 21273033, 21203024, and 21573042) and the Fujian Science and Technology Department (2014J06003 and 2014H6007). S.X. gratefully acknowledges the support of the Recruitment Program of Global Young Experts, Program for New Century Excellent Talents in University (NCET-10-0108), and the Award 'MinJiang Scholar Program' in Fujian Province.en
dc.publisherWiley-Blackwellen
dc.subjectcolumn breakthroughen
dc.subjectmetal-organic frameworksen
dc.subjectopen O donorsen
dc.subjectselective gas adsorptionen
dc.subjectstructural diversityen
dc.titleExtraordinary Separation of Acetylene-Containing Mixtures with Microporous Metal-Organic Frameworks with Open O Donor Sites and Tunable Robustness through Control of the Helical Chain Secondary Building Unitsen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalChemistry - A European Journalen
dc.contributor.institutionFujian Provincial Key Laboratory of Polymer Materials; Fujian Normal University; 32 Shangsan Road Fuzhou 350007 P. R. Chinaen
dc.contributor.institutionNIST Center for Neutron Research; Gaithersburg Maryland 20899-6102 USAen
dc.contributor.institutionInstitute for New Energy Materials & Low-Carbon Technologies; School of Materials Science and Engineering; Tianjin University of Technology; Tianjin 300384 P. R. Chinaen
dc.contributor.institutionDepartment of Chemistry; University of Texas at San Antonio; One UTSA Circle San Antonio Texas 78249-0698 USAen
dc.contributor.institutionVan't Hoff Institute for Molecular Sciences; University of Amsterdam; Science Park 904 Amsterdam 1098 XH The Netherlandsen
kaust.authorZhao, Yunfengen
kaust.authorHan, Yuen
dc.relation.isSupplementedByYao, Z., Zhang, Z., Liu, L., Li, Z., Zhou, W., Zhao, Y., … Xiang, S. (2016). CCDC 1421052: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1jpqdben
dc.relation.isSupplementedByDOI:10.5517/ccdc.csd.cc1jpqdben
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624521en
dc.relation.isSupplementedByYao, Z., Zhang, Z., Liu, L., Li, Z., Zhou, W., Zhao, Y., … Xiang, S. (2016). CCDC 1421054: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1jpqgden
dc.relation.isSupplementedByDOI:10.5517/ccdc.csd.cc1jpqgden
dc.relation.isSupplementedByHANDLE:http://hdl.handle.net/10754/624522en
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