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


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.

SUBMITTER: Gerschel P 

PROVIDER: S-EPMC6504587 | biostudies-literature | 2019 May

REPOSITORIES: biostudies-literature

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Sulfur substitution in a Ni(cyclam) derivative results in lower overpotential for CO<sub>2</sub> reduction and enhanced proton reduction.

Gerschel P P   Warm K K   Farquhar E R ER   Englert U U   Reback M L ML   Siegmund D D   Ray K K   Apfel U-P UP  

Dalton transactions (Cambridge, England : 2003) 20190501 18


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 predomi  ...[more]

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