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Issue 18, 2019
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Sulfur substitution in a Ni(cyclam) derivative results in lower overpotential for CO2 reduction and enhanced proton reduction

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Abstract

The replacement of the opposing nitrogen atoms in 1,4,8,11-tetraazacyclotetradecane (cyclam) with two sulfur atoms in 1,8-dithia-4,11-diazacyclotetradecane (dithiacyclam) enables the electrochemical reduction of protons and CO2via the corresponding nickel(II) complex at more positive potentials. In addition, a 10-fold enhancement in the proton reduction rate of [Ni(dithiacyclam)]2+ relative to [Ni(cylcam)]2+ was observed. The study provides vital insight into Nature's choice of employing predominantly sulfur based ligand platforms in achieving biological proton and CO2 reductions.

Graphical abstract: Sulfur substitution in a Ni(cyclam) derivative results in lower overpotential for CO2 reduction and enhanced proton reduction

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Publication details

The article was received on 30 Nov 2018, accepted on 21 Dec 2018 and first published on 26 Dec 2018


Article type: Paper
DOI: 10.1039/C8DT04740E
Dalton Trans., 2019,48, 5923-5932

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    Sulfur substitution in a Ni(cyclam) derivative results in lower overpotential for CO2 reduction and enhanced proton reduction

    P. Gerschel, K. Warm, E. R. Farquhar, U. Englert, M. L. Reback, D. Siegmund, K. Ray and U.-P. Apfel, Dalton Trans., 2019, 48, 5923
    DOI: 10.1039/C8DT04740E

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