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Issue 12, 2014
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Controlling charge separation in a novel donor–acceptor metal–organic framework via redox modulation

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Abstract

Charge transfer metal–organic frameworks represent a versatile class of multifunctional materials that offer an unprecedented combination of physical properties. The framework [(Zn(DMF))2(TTFTC)(DPNI)] incorporating the donor and acceptor, tetrathiafulvalenetetracarboxylate (TTFTC) and N,N′-di-(4-pyridyl)-1,4,5,8-naphthalenetetracarboxydiimide (DPNI) respectively, exhibits charge transfer by virtue of donor–acceptor interactions within its crystalline structure. This through-space interaction is manifested by the formation of ligand-based radicals in the as-synthesised material and leads to a partial degree of charge separation. Five distinct electronic states of the framework can be accessed using solid state electrochemical and spectroelectrochemical techniques, including for the first time in application to metal–organic frameworks, EPR spectroelectrochemistry (SEC). The degree of charge transfer is controllable via redox modulation and has been quantified using complementary DFT modelling of the charge transfer states.

Graphical abstract: Controlling charge separation in a novel donor–acceptor metal–organic framework via redox modulation

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Publication details

The article was received on 27 May 2014, accepted on 31 Jul 2014 and first published on 04 Aug 2014


Article type: Edge Article
DOI: 10.1039/C4SC01551G
Citation: Chem. Sci., 2014,5, 4724-4728
  • Open access: Creative Commons BY license
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    Controlling charge separation in a novel donor–acceptor metal–organic framework via redox modulation

    C. F. Leong, B. Chan, T. B. Faust and D. M. D'Alessandro, Chem. Sci., 2014, 5, 4724
    DOI: 10.1039/C4SC01551G

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