Zirconium metal-organic frameworks incorporating tetrathiafulvalene linkers: robust and redox-active matrices for in situ confinement of metal nanoparticles.

Chemical Science
Jian SuHong-Cai Zhou

Abstract

Redox-active metal-organic frameworks (MOFs), with highly ordered porous structures and redox tunability, have attracted research interest in the fields of catalysis, energy storage, and electrochemical sensing. However, the chemical lability has limited the application scope of many redox-active MOFs. Herein, we selected stable Zr6 inorganic nodes and redox-active tetrathiafulvalene (TTF)-based linkers to construct two robust, redox-active MOFs, namely compounds 1 ([Zr6(TTFTB)2O8(OH2)8]) and 2 ([Zr6(Me-TTFTB)1.5O4(OH)4(C6H5COO)6]) (TTFTB = tetrathiafulvalene tetrabenzoate; Me-TTFTB = tetrathiafulvalene tetramethylbenzoate). The structure and topology of the MOFs were controlled by tuning the linker conformation through steric effects, resulting in a variety of pore structures from microporous channels (compound 1) to hierarchically micro/mesoporous cages (compound 2). Compound 2 shows high porosity with a BET surface area of 1932 m2 g-1 and strong chemical stability in aqueous solutions with pH ranging from 1 to 12. Furthermore, the reductive TTF moieties allow for in situ generation and stabilization of ultra-small noble metal (Ag, Pd, and Au) nanoparticles by incubating MOFs in the respective metal salt solution. Single crys...Continue Reading

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Methods Mentioned

BETA
X-ray
transmission electron microscopy

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