Issue 18, 2019

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.

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

Supplementary files

Article information

Article type
Paper
Submitted
30 Xim 2018
Accepted
21 Kax 2018
First published
26 Kax 2018

Dalton Trans., 2019,48, 5923-5932

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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