Quest for Highly-connected MOF Platforms: Rare-Earth Polynuclear Clusters Versatility Meets Net Topology Needs.
Type
ArticleAuthors
Alezi, Dalal
Peedikakkal, Abdul Malik P.
Weselinski, Lukasz Jan

Guillerm, Vincent

Belmabkhout, Youssef

Cairns, Amy
Chen, Zhijie

Wojtas, Lukasz
Eddaoudi, Mohamed

KAUST Department
Advanced Membranes and Porous Materials Research CenterChemical Science Program
Functional Materials Design, Discovery and Development (FMD3)
Physical Science and Engineering (PSE) Division
Date
2015-04-17Online Publication Date
2015-04-17Print Publication Date
2015-04-29Permanent link to this record
http://hdl.handle.net/10754/528236
Metadata
Show full item recordAbstract
Gaining control over the assembly of highly porous rare-earth (RE) based metal-organic frameworks (MOFs) remains challenging. Here we report the latest discoveries on our continuous quest for highly-connected nets. The topological exploration based on the non-compatibility of 12-connected RE polynuclear carboxylate-based cluster, points of extension matching the 12 vertices of the cuboctahedron (cuo), with 3-connected organic ligands led to the discovery of two fascinating and highly-connected minimal edge-transitive nets, pek and aea. The reduced symmetry of the employed triangular tricarboxylate ligand, as compared to the prototype highly symmetrical 1,3,5-benzene(tris)benzoic acid guided the concurrent occurrence of nonanuclear [RE9(μ3-OH)12(μ3-O)2(O2C–)12] and hexanuclear [RE6(OH)8(O2C–)8] carboxylate-based clusters as 12-connected and 8-connected molecular building blocks in the structure of a 3-periodic pek-MOF based on a novel (3,8,12)-c trinodal net. The use of a tricarboxylate ligand with modified angles between carboxylate moieties led to the formation of a second MOF containing solely nonanuclear clusters and exhibiting once more a novel and a highly-connected (3,12,12)-c trinodal net with aea topology. Notably, it is the first time that RE-MOFs with double six-membered ring (d6R) secondary building units are isolated, representing therefore a critical step forward toward the design of novel and highly coordinated materials using the supermolecular building layer approach while considering the d6Rs as building pillars. Lastly, the potential of these new MOFs for gas separation/storage was investigated by performing gas adsorption studies of various probe gas molecules over a wide range of pressures. Noticeably, pek-MOF-1 showed excellent volumetric CO2 and CH4 uptakes at high pressures.Citation
Quest for Highly-connected MOF Platforms: Rare-Earth Polynuclear Clusters Versatility Meets Net Topology Needs. 2015:150407200837004 Journal of the American Chemical SocietyPublisher
American Chemical Society (ACS)PubMed ID
25851127Additional Links
http://pubs.acs.org/doi/abs/10.1021/jacs.5b00450Relations
Is Supplemented By:- [Dataset]
Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410819: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc298. DOI: 10.5517/cc1jc298 HANDLE: 10754/624447 - [Dataset]
Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410820: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc2b9. DOI: 10.5517/cc1jc2b9 HANDLE: 10754/624448 - [Dataset]
Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410821: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc2cb. DOI: 10.5517/cc1jc2cb HANDLE: 10754/624449 - [Dataset]
Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410822: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc2dc. DOI: 10.5517/cc1jc2dc HANDLE: 10754/624450 - [Dataset]
Alezi, D., Peedikakkal, A. M. P., Weseliński, Ł. J., Guillerm, V., Belmabkhout, Y., Cairns, A. J., … Eddaoudi, M. (2015). CCDC 1410823: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/cc1jc2fd. DOI: 10.5517/cc1jc2fd HANDLE: 10754/624451
ae974a485f413a2113503eed53cd6c53
10.1021/jacs.5b00450
Scopus Count
Related articles
- Applying the Power of Reticular Chemistry to Finding the Missing alb-MOF Platform Based on the (6,12)-Coordinated Edge-Transitive Net.
- Authors: Chen Z, Weseliński ŁJ, Adil K, Belmabkhout Y, Shkurenko A, Jiang H, Bhatt PM, Guillerm V, Dauzon E, Xue DX, O'Keeffe M, Eddaoudi M
- Issue date: 2017 Mar 1
- Enriching the Reticular Chemistry Repertoire with Minimal Edge-Transitive Related Nets: Access to Highly Coordinated Metal-Organic Frameworks Based on Double Six-Membered Rings as Net-Coded Building Units.
- Authors: Chen Z, Thiam Z, Shkurenko A, Weselinski LJ, Adil K, Jiang H, Alezi D, Assen AH, O'Keeffe M, Eddaoudi M
- Issue date: 2019 Dec 26
- Minimal edge-transitive nets for the design and construction of metal-organic frameworks.
- Authors: Chen Z, Jiang H, O'Keeffe M, Eddaoudi M
- Issue date: 2017 Sep 8
- The Importance of Highly Connected Building Units in Reticular Chemistry: Thoughtful Design of Metal-Organic Frameworks.
- Authors: Guillerm V, Eddaoudi M
- Issue date: 2021 Sep 7
- The Highly Connected MOFs Constructed from Nonanuclear and Trinuclear Lanthanide-Carboxylate Clusters: Selective Gas Adsorption and Luminescent pH Sensing.
- Authors: Li YJ, Wang YL, Liu QY
- Issue date: 2017 Feb 20