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Article ; Online: Reticular Synthesis of Flexible Rare-Earth Metal-Organic Frameworks: Control of Structural Dynamics and Sorption Properties Through Ligand Functionalization.

Loukopoulos, Edward / Angeli, Giasemi K / Tsangarakis, Constantinos / Traka, Eleni / Froudas, Konstantinos G / Trikalitis, Pantelis N

Chemistry (Weinheim an der Bergstrasse, Germany)

2023 Volume 30, Issue 4, Page(s) e202302709

Abstract: An exciting direction in metal-organic frameworks involves the design and synthesis of flexible structures which can reversibly adapt their structure when triggered by external stimuli. Controlling the extent and nature of response in such solids is ... ...

Abstract	An exciting direction in metal-organic frameworks involves the design and synthesis of flexible structures which can reversibly adapt their structure when triggered by external stimuli. Controlling the extent and nature of response in such solids is critical in order to develop custom dynamic materials for advanced applications. Towards this, it is highly important to expand the diversity of existing flexible MOFs, generating novel materials and gain an in-depth understanding of the associated dynamic phenomena, eventually unlocking key structure-property relationships. In the present work, we successfully utilized reticular chemistry for the construction of two novel series of highly crystalline, flexible rare-earth MOFs, RE-thc-MOF-2 and RE-teb-MOF-1. Extensive single-crystal to single-crystal structural analyses coupled with detailed gas and vapor sorption studies, shed light onto the unique responsive behavior. The development of these series is related to the reported RE-thc-MOF-1 solids which were found to display a unique continuous breathing and gas-trapping property. The synthesis of RE-thc-MOF-2 and RE-teb-MOF-1 materials represents an important milestone as they provide important insights into the key factors that control the responsive properties of this fascinating family of flexible materials and demonstrates that it is possible to control their dynamic behavior and the associated gas and vapor sorption properties.
Language	English
Publishing date	2023-11-27
Publishing country	Germany
Document type	Journal Article
ZDB-ID	1478547-X
ISSN	1521-3765 ; 0947-6539
ISSN (online)	1521-3765
ISSN	0947-6539
DOI	10.1002/chem.202302709
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Article ; Online: Accessing 14-Connected Nets: Continuous Breathing, Hydrophobic Rare-Earth Metal Organic Frameworks Based on 14-c Hexanuclear Clusters with High Affinity for Non-Polar Vapors.

Loukopoulos, Edward / Angeli, Giasemi K / Kouvidis, Konstantinos / Tsangarakis, Constantinos / Trikalitis, Pantelis N

ACS applied materials & interfaces

2022 Volume 14, Issue 19, Page(s) 22242–22251

Abstract: Highly connected metal organic frameworks (MOFs) in which at least one building block has connectivity higher than twelve are very rare and much desirable. We report here the first examples of isostructural 14-connected MOFs, RE- ...

Abstract	Highly connected metal organic frameworks (MOFs) in which at least one building block has connectivity higher than twelve are very rare and much desirable. We report here the first examples of isostructural 14-connected MOFs, RE-
Language	English
Publishing date	2022-05-10
Publishing country	United States
Document type	Journal Article
ISSN	1944-8252
ISSN (online)	1944-8252
DOI	10.1021/acsami.2c05961
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Article ; Online: Expanding the Reticular Chemistry Building Block Library toward Highly Connected Nets: Ultraporous MOFs Based on 18-Connected Ternary, Trigonal Prismatic Superpolyhedra.

Froudas, Konstantinos G / Vassaki, Maria / Papadopoulos, Konstantinos / Tsangarakis, Constantinos / Chen, Xu / Shepard, William / Fairen-Jimenez, David / Tampaxis, Christos / Charalambopoulou, Georgia / Steriotis, Theodore A / Trikalitis, Pantelis N

Journal of the American Chemical Society

2024 Volume 146, Issue 13, Page(s) 8961–8970

Abstract: The chemistry of metal-organic frameworks (MOFs) continues to expand rapidly, providing materials with diverse structures and properties. The reticular chemistry approach, where well-defined structural building blocks are combined together to form ... ...

Abstract	The chemistry of metal-organic frameworks (MOFs) continues to expand rapidly, providing materials with diverse structures and properties. The reticular chemistry approach, where well-defined structural building blocks are combined together to form crystalline open framework solids, has greatly accelerated the discovery of new and important materials. However, its full potential toward the rational design of MOFs relies on the availability of highly connected building blocks because these greatly reduce the number of possible structures. Toward this, building blocks with connectivity greater than 12 are highly desirable but extremely rare. We report here the discovery of novel 18-connected, trigonal prismatic, ternary building blocks (
Language	English
Publishing date	2024-03-01
Publishing country	United States
Document type	Journal Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.3c12679
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Article: Continuous Breathing Rare-Earth MOFs Based on Hexanuclear Clusters with Gas Trapping Properties

Angeli, Giasemi K. / Loukopoulos, Edward / Kouvidis, Konstantinos / Bosveli, Artemis / Tsangarakis, Constantinos / Tylianakis, Emmanuel / Froudakis, George / Trikalitis, Pantelis N.

Journal of the American Chemical Society. 2021 June 29, v. 143, no. 27

2021

Abstract: Guest responsive porous materials represent an important and fascinating class of multifunctional solids that have attracted considerable attention in recent years. An understanding of how these structures form is essential toward their rational design, ... ...

Abstract	Guest responsive porous materials represent an important and fascinating class of multifunctional solids that have attracted considerable attention in recent years. An understanding of how these structures form is essential toward their rational design, which is a prerequisite for the development of tailor-made materials for advanced applications. We herein report a novel series of stable rare-earth (RE) MOFs that show a rare continuous breathing behavior and an unprecedented gas-trapping property. We used an asymmetric 4-c tetratopic carboxylate-based organic ligand that is capable of affording highly crystalline materials upon controlled reaction with RE cations. These MOFs, denoted as RE-thc-MOF-1 (RE: Y³⁺, Sm³⁺, Eu³⁺, Tb³⁺, Dy³⁺, Ho³⁺, and Er³⁺), feature hexanuclear RE₆ clusters that display a highly unusual connectivity and serve as unique 8-c hemi-cuboctahedral secondary building block, resulting in a new (3,3,8)-c thc topology. Extensive single-crystal to single-crystal structural analyses coupled with detailed gas (N₂, Ar, Kr, CO₂, CH₄, and Xe) and vapor (EtOH, CH₃CN, C₆H₆, and C₆H₁₄) sorption studies, supported by accurate theoretical calculations, shed light onto the unique swelling behavior. The results reveal a synergistic action involving steric effects, associated with coordinated solvent molecules and 2-fluorobenzoate (2-FBA) nonbridging ligands, as well as cation–framework electrostatic interactions. We were able to probe the individual role of the coordinated solvent molecules and 2-FBA ligands and found that both cooperatively control the gas-breathing and -trapping properties, while 2-FBA controls the vapor adsorption selectivity. These findings provide unique opportunities toward the design and development of tunable RE-based flexible MOFs with tailor-made properties.
Keywords	adsorption ; carbon dioxide ; ligands ; solvents ; synergism ; topology ; vapors
Language	English
Dates of publication	2021-0629
Size	p. 10250-10260.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.1c03762
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Water-Stable

Tsangarakis, Constantinos / Azmy, Ali / Tampaxis, Christos / Zibouche, Nourdine / Klontzas, Emmanuel / Tylianakis, Emmanuel / Froudakis, George E / Steriotis, Theodore / Spanopoulos, Ioannis / Trikalitis, Pantelis N

Inorganic chemistry

2023 Volume 62, Issue 14, Page(s) 5496–5504

Abstract: We utilized ... ...

Abstract	We utilized the
Language	English
Publishing date	2023-03-28
Publishing country	United States
Document type	Journal Article
ZDB-ID	1484438-2
ISSN	1520-510X ; 0020-1669
ISSN (online)	1520-510X
ISSN	0020-1669
DOI	10.1021/acs.inorgchem.2c04483
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Article: Remarkable Structural Diversity between Zr/Hf and Rare-Earth MOFs via Ligand Functionalization and the Discovery of Unique (4, 8)-c and (4, 12)-connected Frameworks

Angeli, Giasemi K / Batzavali, Danai / Mavronasou, Katerina / Tsangarakis, Constantinos / Stuerzer, Tobias / Ott, Holger / Trikalitis, Pantelis N

Journal of the American Chemical Society. 2020 Aug. 26, v. 142, no. 37

2020

Abstract: Ligand modification in MOFs provides great opportunities not only for the development of functional materials with new or enhanced properties but also for the discovery of novel structures. We report here that a sulfone-functionalized tetrahedral ... ...

Abstract	Ligand modification in MOFs provides great opportunities not only for the development of functional materials with new or enhanced properties but also for the discovery of novel structures. We report here that a sulfone-functionalized tetrahedral carboxylate-based ligand is capable of directing the formation of new and fascinating MOFs when combined with Zr⁴⁺/Hf⁴⁺ and rare-earth metal cations (RE) with improved gas-sorption properties. In particular, the resulting M-flu-SO₂ (M: Zr, Hf) materials display a new type of the augmented flu-a net, which is different as compared to the flu-a framework formed by the nonfunctionalized tetrahedral ligand. In terms of properties, a remarkable increase in the CO₂ uptake is observed that reaches 76.6% and 61.6% at 273 and 298 K and 1 bar, respectively. When combined with REs, the sulfone-modified linker affords novel MOFs, RE-hpt-MOF-1 (RE: Y³⁺, Ho³⁺, Er³⁺), which displays a fascinating (4, 12)-coordinated hpt net, based on nonanuclear [RE₉(μ₃-Ο)₂(μ₃-ΟΗ)₁₂(−COO)₁₂] clusters that serve as hexagonal prismatic building blocks. In the absence of the sulfone groups, we discovered that the tetrahedral linker directs the formation of new RE-MOFs, RE-ken-MOF-1 (RE: Y³⁺, Ho³⁺, Er³⁺, Yb³⁺), that display an unprecedented (4, 8)-coordinated ken net based on nonanuclear RE₉-clusters, to serve as bicapped trigonal prismatic building units. Successful activation of the representative member Y-ken-MOF-1 reveals a high BET surface area and total pore volume reaching 2621 m² g–¹ and 0.95 cm³ g–¹, respectively. These values are the highest among all RE MOFs based on nonanuclear clusters and some of the highest in the entire RE family of MOFs. The present work uncovers a unique structural diversity existing between Zr/Hf and RE-based MOFs that demonstrates the crucial role of linker design. In addition, the discovery of the new RE-hpt-MOF-1 and RE-ken-MOF-1 families of MOFs highlights the great opportunities existing in RE-MOFs in terms of structural diversity that could lead to novel materials with new properties.
Keywords	carbon dioxide ; ligands ; surface area
Language	English
Dates of publication	2020-0826
Size	p. 15986-15994.
Publishing place	American Chemical Society
Document type	Article
Note	NAL-AP-2-clean
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.0c07081
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Continuous Breathing Rare-Earth MOFs Based on Hexanuclear Clusters with Gas Trapping Properties.

Angeli, Giasemi K / Loukopoulos, Edward / Kouvidis, Konstantinos / Bosveli, Artemis / Tsangarakis, Constantinos / Tylianakis, Emmanuel / Froudakis, George / Trikalitis, Pantelis N

Journal of the American Chemical Society

2021 Volume 143, Issue 27, Page(s) 10250–10260

Abstract	Guest responsive porous materials represent an important and fascinating class of multifunctional solids that have attracted considerable attention in recent years. An understanding of how these structures form is essential toward their rational design, which is a prerequisite for the development of tailor-made materials for advanced applications. We herein report a novel series of stable rare-earth (RE) MOFs that show a rare continuous breathing behavior and an unprecedented gas-trapping property. We used an asymmetric 4-c tetratopic carboxylate-based organic ligand that is capable of affording highly crystalline materials upon controlled reaction with RE cations. These MOFs, denoted as RE-
Language	English
Publishing date	2021-06-29
Publishing country	United States
Document type	Journal Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.1c03762
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Remarkable Structural Diversity between Zr/Hf and Rare-Earth MOFs via Ligand Functionalization and the Discovery of Unique (4, 8)-c and (4, 12)-connected Frameworks.

Angeli, Giasemi K / Batzavali, Danai / Mavronasou, Katerina / Tsangarakis, Constantinos / Stuerzer, Tobias / Ott, Holger / Trikalitis, Pantelis N

Journal of the American Chemical Society

2020 Volume 142, Issue 37, Page(s) 15986–15994

Abstract	Ligand modification in MOFs provides great opportunities not only for the development of functional materials with new or enhanced properties but also for the discovery of novel structures. We report here that a sulfone-functionalized tetrahedral carboxylate-based ligand is capable of directing the formation of new and fascinating MOFs when combined with Zr
Language	English
Publishing date	2020-09-04
Publishing country	United States
Document type	Journal Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.0c07081
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Reticular Synthesis of HKUST-like tbo-MOFs with Enhanced CH4 Storage.

Spanopoulos, Ioannis / Tsangarakis, Constantinos / Klontzas, Emmanuel / Tylianakis, Emmanuel / Froudakis, George / Adil, Karim / Belmabkhout, Youssef / Eddaoudi, Mohamed / Trikalitis, Pantelis N

Journal of the American Chemical Society

2016 Volume 138, Issue 5, Page(s) 1568–1574

Abstract: Successful implementation of reticular chemistry using a judiciously designed rigid octatopic carboxylate organic linker allowed the construction of expanded HKUST-1-like tbo-MOF series with intrinsic strong CH4 adsorption sites. The Cu-analogue ... ...

Abstract	Successful implementation of reticular chemistry using a judiciously designed rigid octatopic carboxylate organic linker allowed the construction of expanded HKUST-1-like tbo-MOF series with intrinsic strong CH4 adsorption sites. The Cu-analogue displayed a concomitant enhancement of the gravimetric and volumetric surface area with the highest reported CH4 uptake among the tbo family, comparable to the best performing metal organic frameworks (MOFs) for CH4 storage. The corresponding gravimetric (BET) and volumetric surface areas of 3971 m(2) g(-1) and 2363 m(2) cm(-3) represent an increase of 115% and 47%, respectively, in comparison to the corresponding values for the prototypical HKUST-1 (tbo-MOF-1), and are 42% and 20% higher than that of tbo-MOF-2. High-pressure methane adsorption isotherms revealed a high total gravimetric and volumetric CH4 uptakes, reaching 372 cm(3) (STP) g(-1) and 221 cm(3) (STP) cm(-3), respectively, at 85 bar and 298 K. The corresponding working capacities between 5 and 80 bar were found to be 294 cm(3) (STP) g(-1) and 175 cm(3) (STP) cm(-3) and are placed among the best performing MOFs for CH4 storage particularly at relatively low temperature. To gain insight on the mechanism accounting for the resultant enhanced CH4 storage capacity, molecular simulation study was performed and revealed the presence of very strong CH4 adsorption sites near the organic linker with similar adsorption energetics as the open metal sites. The present findings support the potential of tbo-MOFs based on the supermolecular building layer (SBL) approach as an ideal platform to further enhance the CH4 storage capacity via expansion and functionalization of the quadrangular pillars.
Language	English
Publishing date	2016-02-10
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.5b11079
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Article ; Online: Reticular Chemistry at Its Best: Directed Assembly of Hexagonal Building Units into the Awaited Metal-Organic Framework with the Intricate Polybenzene Topology, pbz-MOF.

Alezi, Dalal / Spanopoulos, Ioannis / Tsangarakis, Constantinos / Shkurenko, Aleksander / Adil, Karim / Belmabkhout, Youssef / O Keeffe, Michael / Eddaoudi, Mohamed / Trikalitis, Pantelis N

Journal of the American Chemical Society

2016 Volume 138, Issue 39, Page(s) 12767–12770

Abstract: The ability to direct the assembly of hexagonal building units offers great prospective to construct the awaited and looked-for hypothetical polybenzene (pbz) or "cubic graphite" structure, described 70 years ago. Here, we demonstrate the successful use ... ...

Abstract	The ability to direct the assembly of hexagonal building units offers great prospective to construct the awaited and looked-for hypothetical polybenzene (pbz) or "cubic graphite" structure, described 70 years ago. Here, we demonstrate the successful use of reticular chemistry as an appropriate strategy for the design and deliberate construction of a zirconium-based metal-organic framework (MOF) with the intricate pbz underlying net topology. The judicious selection of the perquisite hexagonal building units, six connected organic and inorganic building blocks, allowed the formation of the pbz-MOF-1, the first example of a Zr(IV)-based MOF with pbz topology. Prominently, pbz-MOF-1 is highly porous, with associated pore size and pore volume of 13 Å and 0.99 cm
Language	English
Publishing date	2016-10-05
Publishing country	United States
Document type	Journal Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.6b08176
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