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Royal Society of Chemistry, Faraday Discussions, (183), p. 147-160, 2015

DOI: 10.1039/c5fd00071h

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Improving the efficiency of electrochemical CO2 reduction using immobilized manganese complexes

Journal article published in 2015 by James J. Walsh ORCID, Charlotte L. Smith, Gaia Neri, George F. S. Whitehead, Craig M. Robertson, Alexander J. Cowan ORCID
This paper was not found in any repository, but could be made available legally by the author.
This paper was not found in any repository, but could be made available legally by the author.

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Abstract

Immobilization of [Mn(bpy)(CO)3Br], (1) and [Mn(bpy(tBu)2)(CO)3Br] (2, where (bpy(tBu)2) = 4,4′-di-tert-butyl-2,2′-bipyridine) in Nafion/multi-walled carbon nanotubes (MWCNT) on glassy carbon yielded highly active electrodes for the reduction of CO2 to CO in aqueous solutions at pH 7. Films incorporating 2 have significantly improved selectivity towards CO2, with CO : H2 ∼ 1 at −1.4 V vs. SCE, exceeding that for the previously reported 1/MWCNT/Nafion electrode. Furthermore, we report the synthesis and subsequent electrochemical characterization of two new substituted Mn(i) bipyridine complexes, [Mn(bpy(COOH)2)(CO)3Br] (3) and [Mn(bpy(OH)2)(CO)3Br] (4) (where (bpy(COOH)2) = 4,4′-di-carboxy-2,2′-bipyridine and (bpy(OH)2) = 4,4′-di-hydroxy-2,2′-bipyridine). Both 3 and 4 were found to have some activity towards CO2 in acetonitrile solutions; however once immobilized in Nafion membranes CO2 reduction was found to not occur at significant levels.