Publication: Topological transplantations in MOFs – Nature Chemistry

My main post-doctoral project are finally published ! After a long time working, designing, and writing up, the paper is now out in the prestigious journal Nature Chemistry. This nice work is also highlighted on the cover of the journal. (get the article as pdf)

Nature Chemistry cover (August 2014) highlighting the gea-MOF paper

I must thank my colleague and friend Łukasz, the great organic chemist who made the crazy ligand become real !

Following the breakthrough results recently published in J. Am. Chem. Soc. by my colleague Dongxu Xue, about the synthesis of various fcu-MOFs, based on rare earths (RE) inorganic clusters, I explored the combination of a triangular ligand and RE, in the presence of fluorinated modulator, and isolated a new highly connected RE nonanuclear cluster. This cluster is surrounded by eighteen 3-connected ligands to form MOF with a highly connected (3,18)-c net, gea topology (gea: guillerm, eddaoudi, net a). This gea-MOF-1 is highly porous, thermally stable, catalytically active for the synthesis of cyclic carbonates, and shows great promises for the separation of hydrocarbons.

topological exploration2.png
Topological exploration followed to discover gea-MOF-1 and the related gea net (Adapted from Nature Chem).
The unique expertise of the FMD3 group in topological analysis and MOF design was very helpful to recognize that the gea net, qualified by Prof. Mike O’Keeffe as an “exceptionally interesting net”, can be utilized as a blueprint for the rational design of gigantic MOFs, utilizing the Supermolecular Building Blocks (SBB) approach to replace the inorganic 18-c cluster by an open metal-organic polyhedron (MOP).
Indeed, such a MOP has already been described as discrete entity, and results from the assembly of two types of bent ligands (6×90o and 120o angles) and 4-connected Cu paddle wheels. Interestingly, the unveilment of the gea net now provides the required information to link them together in a MOF for the first time. By the careful geometrical analysis, the FMD3 team designed and synthesized an asymmetric hexacarboxylic ligand containing the appropriate angles (1×90o and 2×120o). As expected, its combination with cupper paddle wheels resulted in the formation of gea-MOF-2, the first SBB based MOF with the same general gea topology.

Unambiguously, this report shows that MOF design finally became true!


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