scholarly journals Exploiting Large-Pore Metal-Organic Frameworks for Separations through Entropic Molecular Mechanisms

ChemPhysChem ◽  
2015 ◽  
Vol 16 (10) ◽  
pp. 2046-2067 ◽  
Author(s):  
Ariana Torres-Knoop ◽  
David Dubbeldam
Keyword(s):  
Molecular Mechanisms ◽  
Metal Organic Frameworks ◽  
Large Pore ◽  
Metal Organic

Large-Pore Apertures in a Series of Metal-Organic Frameworks

Science ◽  
2012 ◽  
Vol 336 (6084) ◽  
pp. 1018-1023 ◽  
Author(s):  
H. Deng ◽  
S. Grunder ◽  
K. E. Cordova ◽  
C. Valente ◽  
H. Furukawa ◽  
...  
Keyword(s):  
Metal Organic Frameworks ◽  
Large Pore ◽  
Metal Organic

scholarly journals Predicting the Features of Methane Adsorption in Large Pore Metal-Organic Frameworks for Energy Storage

Nanomaterials ◽  
2018 ◽  
Vol 8 (10) ◽  
pp. 818 ◽  
Author(s):  
George Manos ◽  
Lawrence Dunne
Keyword(s):  
Gas Adsorption ◽  
Metal Organic Frameworks ◽  
Gas Storage ◽  
Methane Adsorption ◽  
Energy Applications ◽  
Adsorbed Gas ◽  
Theoretical Approaches ◽  
Large Pore ◽  
Metal Organic ◽  
Computer Simulation Studies

Currently, metal-organic frameworks (MOFs) are receiving significant attention as part of an international push to use their special properties in an extensive variety of energy applications. In particular, MOFs have exceptional potential for gas storage especially for methane and hydrogen for automobiles. However, using theoretical approaches to investigate this important problem presents various difficulties. Here we present the outcomes of a basic theoretical investigation into methane adsorption in large pore MOFs with the aim of capturing the unique features of this phenomenon. We have developed a pseudo one-dimensional statistical mechanical theory of adsorption of gas in a MOF with both narrow and large pores, which is solved exactly using a transfer matrix technique in the Osmotic Ensemble (OE). The theory effectively describes the distinctive features of adsorption of gas isotherms in MOFs. The characteristic forms of adsorption isotherms in MOFs reflect changes in structure caused by adsorption of gas and compressive stress. Of extraordinary importance for gas storage for energy applications, we find two regimes of Negative gas adsorption (NGA) where gas pressure causes the MOF to transform from the large pore to the narrow pore structure. These transformations can be induced by mechanical compression and conceivably used in an engine to discharge adsorbed gas from the MOF. The elements which govern NGA in MOFs with large pores are identified. Our study may help guide the difficult program of work for computer simulation studies of gas storage in MOFs with large pores.

scholarly journals Elucidating CO2 Chemisorption in Diamine-Appended Metal–Organic Frameworks

2018 ◽  
Author(s):  
Alexander C. Forse ◽  
Phillip J. Milner ◽  
Jung-Hoon Lee ◽  
Halle N. Redfearn ◽  
Julia Oktawiec ◽  
...  
Keyword(s):  
Carbon Capture ◽  
Density Functional ◽  
Molecular Mechanisms ◽  
Metal Organic Frameworks ◽  
Carbamic Acid ◽  
Co2 Uptake ◽  
Functional Theory ◽  
Ammonium Carbamate ◽  
Co2 Chemisorption ◽  
Metal Organic

The widespread deployment of carbon capture and sequestration as a climate change mitigation strategy could be facilitated by the development of more energy-efficient adsorbents. Diamine-appended metal–organic frameworks of the type diamine–M2(dobpdc) (M = Mg, Mn, Fe, Co, Ni, Zn; dobpdc4− = 4,4′-dioxidobiphenyl-3,3′-dicarboxylate) have shown promise for carbon capture applications, although questions remain regarding the molecular mechanisms of CO2 uptake in these materials. Here, we leverage the crystallinity and tunability of this class of frameworks to perform a comprehensive study of CO2 chemisorption. Using multinuclear nuclear magnetic resonance (NMR) spectroscopy experiments and van der Waals-corrected density functional theory (DFT) calculations for thirteen diamine–M2(dobpdc) variants, we demonstrate that the canonical CO2 chemisorption products—ammonium carbamate chains and carbamic acid pairs—can be readily distinguished, and that ammonium carbamate chain formation dominates for diamine–Mg2(dobpdc) materials. In addition, we elucidate a new chemisorption mechanism in the material dmpn Mg2(dobpdc) (dmpn = 2,2-dimethyl-1,3-diaminopropane), which involves formation of a 1:1 mixture of ammonium carbamate and carbamic acid and accounts for the unusual adsorption properties of this material. Finally, we show that the presence of water plays an important role in directing the mechanisms for CO2 uptake in diamine–M2(dobpdc) materials. Overall, our combined NMR and DFT approach enables a thorough depiction and understanding of CO2 adsorption within diamine–M2(dobpdc) compounds, which may aid similar studies in other amine-functionalized adsorbents in the future.

Thermodynamics of the structural transition in metal–organic frameworks

2016 ◽  
Vol 45 (10) ◽  
pp. 4274-4282 ◽  
Author(s):  
J. Rodriguez ◽  
I. Beurroies ◽  
M.-V. Coulet ◽  
P. Fabry ◽  
T. Devic ◽  
...  
Keyword(s):  
Structural Transition ◽  
Metal Organic Frameworks ◽  
Thermodynamic Study ◽  
Large Pore ◽  
Metal Organic

A thermodynamic study of the structural large-pore (LP) to narrow pore (NP) transition in various Metal Organic Frameworks (MOFs) is presented.

Large-pore mesoporous Mn3O4 crystals derived from metal–organic frameworks

2013 ◽  
Vol 49 (99) ◽  
pp. 11695 ◽  
Author(s):  
Li Peng ◽  
Jianling Zhang ◽  
Zhimin Xue ◽  
Buxing Han ◽  
Jianshen Li ◽  
...  
Keyword(s):  
Metal Organic Frameworks ◽  
Large Pore ◽  
Metal Organic

Strategies for Characterization of Large-Pore Metal-Organic Frameworks by Combined Experimental and Computational Methods

2009 ◽  
Vol 21 (20) ◽  
pp. 4768-4777 ◽  
Author(s):  
Youn-Sang Bae ◽  
David Dubbeldam ◽  
Andrew Nelson ◽  
Krista S. Walton ◽  
Joseph T. Hupp ◽  
...  
Keyword(s):  
Computational Methods ◽  
Metal Organic Frameworks ◽  
Large Pore ◽  
Metal Organic
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