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Lee, Ji U,John C. Eklund,Robert A. W. Dryfe,Richard G. Compton Korean Chemical Society 1996 Bulletin of the Korean Chemical Society Vol.17 No.2
Two redox processes of methyl viologen (+2/+, +/0) in acetonitrile were investigated by using channel electrode voltammetric and in situ electrochemical ESR methods. Two separated unequal plateau currents of the first (+2/+) and second (+/0) redox processes of the viologen were observed in the channel electrode voltammograms and showed a cube-root depedndence on the electrolyte flow rate, respectively. The simple Levich analysis resulted in two different diffusion coefficients of $D_{+2}=2.2{\times}10^{-5}\;cm^2/s$ and $D_+=3.0{\times}10^{-5}cm^2/s$ from the limiting currents. In situ electrochemical ESR studies were performed for the monocation radicals generated at the potentials of the two plateau currents in the electrolyte flow range $1.3{\times}10^{-1}{\geq}v_f{\geq}2.7{\times}10^{-3}\;cm^3/s$. Backward implicitfinite difference method was employed to simulate the electrochemical kinetic problem of two sequential electron transfers ($MV^{+2}+e{\leftrightarrows}MV^+,\;MV^{+}+e{\leftrightarrows}MV^0$) coupled with reversible comproportionation ($MV^{2+}+MV^0{{\leftrightarrows}^{k_f}_{k_b}}2MV^+$). $k_f$ was found to be greater than ($10^6M^{-1}s^{-1}.
Electronic structure design for nanoporous, electrically conductive zeolitic imidazolate frameworks
Butler, Keith T.,Worrall, Stephen D.,Molloy, Christopher D.,Hendon, Christopher H.,Attfield, Martin P.,Dryfe, Robert A. W.,Walsh, Aron Royal Society of Chemistry 2017 Journal of Materials Chemistry C Vol.5 No.31
<▼1><P>Electronic structure calculations are used to develop design rules for enhanced electrical conductivity in zeolitic imidazolate frameworks.</P></▼1><▼2><P>Electronic structure calculations are used to develop design rules for enhanced electrical conductivity in zeolitic imidazolate frameworks. The electrical resistivity of Co<SUP>2+</SUP> based zeolitic imidazolate frameworks has previously been found to be ∼1000 times lower than that of Zn<SUP>2+</SUP> based materials. The electrical conductivity of the frameworks can also be tuned by ligand molecule selection. Using density functional theory calculations, this controllable electrical conductivity is explained in terms of tuneable conduction band edge character, with calculations revealing the improved hybridisation and extended band character of the Co<SUP>2+</SUP> frameworks. The improvements in the methylimidazolate frameworks are understood in terms of improved frontier orbital matching between metal and ligand. The modular tuneability and previously demonstrated facile synthesis provides a route to rational design of stable framework materials for electronic applications. By outlining these design principles we provide a route to the future development of stable, electrically conductive zeolitic imidazolate frameworks.</P></▼2>