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Synthesis and Characterization of Functionalized Metal-organic Frameworks

Synthesis and Characterization of Functionalized Metal-organic Frameworks

Published on: September 5, 2014

Modifying cage structures in metal-organic polyhedral frameworks for H2 storage.

Yong Yan¹, Alexander J Blake, William Lewis

¹School of Chemistry, University of Nottingham, University Park, Nottingham NG7 2RD, UK.

Chemistry (Weinheim an Der Bergstrasse, Germany)

|September 8, 2011

Summary

Three new metal-organic frameworks (NOTT-113, NOTT-114, NOTT-115) exhibit high surface areas and significant hydrogen storage capacities. Functionalizing cage walls with aromatic rings enhances hydrogen interactions, with NOTT-115 showing the highest uptake.

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Area of Science:

Materials Science
Chemistry
Nanotechnology

Background:

Metal-organic frameworks (MOFs) are porous materials with potential applications in gas storage.
Developing MOFs with tailored pore environments is crucial for optimizing gas adsorption properties.
Isostructural MOFs allow for systematic studies of structure-property relationships.

Purpose of the Study:

To synthesize and characterize three isostructural metal-organic polyhedral cage-based frameworks (NOTT-113, NOTT-114, NOTT-115).
To investigate the effect of functional group modification on hydrogen adsorption properties.
To evaluate the hydrogen storage capacity and binding interactions within these novel frameworks.

Main Methods:

Solvothermal synthesis combining hexacarboxylate isophthalate linkers with {Cu(2)(RCOO)(4)} paddlewheels.
Solvent exchange and thermal activation to generate desolvated framework materials.
Gas adsorption analysis (BET surface area, H2 uptake at 77 K and 60 bar).
Calorimetric measurements to determine heats of adsorption (Qst).

Main Results:

Three isostructural frameworks (NOTT-113, NOTT-114, NOTT-115) with cuboctahedral cages were successfully synthesized.
Desolvated materials exhibited high BET surface areas (2970–3424 m²/g).
Hydrogen uptake capacities ranged from 6.7 wt% to 7.5 wt% at 77 K and 60 bar, with NOTT-115 showing the highest uptake.
Heats of adsorption indicated that triphenylamine functionalization in NOTT-115 enhances H2/framework interactions.

Conclusions:

The functionalization of metal-organic framework cage walls significantly influences hydrogen adsorption.
NOTT-115, featuring a triphenylamine moiety, demonstrates superior hydrogen storage capacity and binding affinity.
These findings highlight the potential of rationally designed MOFs for efficient hydrogen storage applications.