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Turning it off! Disfavouring hydrogen evolution to enhance selectivity for CO production during homogeneous CO2 reduction by cobalt-terpyridine complexes.


ABSTRACT: Understanding the activity and selectivity of molecular catalysts for CO2 reduction to fuels is an important scientific endeavour in addressing the growing global energy demand. Cobalt-terpyridine compounds have been shown to be catalysts for CO2 reduction to CO while simultaneously producing H2 from the requisite proton source. To investigate the parameters governing the competition for H+ reduction versus CO2 reduction, the cobalt bisterpyridine class of compounds is first evaluated as H+ reduction catalysts. We report that electronic tuning of the ancillary ligand sphere can result in a wide range of second-order rate constants for H+ reduction. When this class of compounds is next submitted to CO2 reduction conditions, a trend is found in which the less active catalysts for H+ reduction are the more selective towards CO2 reduction to CO. This represents the first report of the selectivity of a molecular system for CO2 reduction being controlled through turning off one of the competing reactions. The activities of the series of catalysts are evaluated through foot-of-the-wave analysis and a catalytic Tafel plot is provided.

SUBMITTER: Elgrishi N 

PROVIDER: S-EPMC5489026 | biostudies-literature | 2015 Apr

REPOSITORIES: biostudies-literature

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Turning it off! Disfavouring hydrogen evolution to enhance selectivity for CO production during homogeneous CO<sub>2</sub> reduction by cobalt-terpyridine complexes.

Elgrishi Noémie N   Chambers Matthew B MB   Fontecave Marc M  

Chemical science 20150218 4


Understanding the activity and selectivity of molecular catalysts for CO<sub>2</sub> reduction to fuels is an important scientific endeavour in addressing the growing global energy demand. Cobalt-terpyridine compounds have been shown to be catalysts for CO<sub>2</sub> reduction to CO while simultaneously producing H<sub>2</sub> from the requisite proton source. To investigate the parameters governing the competition for H<sup>+</sup> reduction <i>versus</i> CO<sub>2</sub> reduction, the cobalt b  ...[more]

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