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Issue 28, 2018
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Mechanisms of catalytic reduction of CO2 with heme and nonheme metal complexes

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Abstract

The catalytic conversion of CO2 into valuable chemicals and fuels has attracted increasing attention, providing a promising route for mitigating the greenhouse effect of CO2 and also meeting the global energy demand. Among many homogeneous and heterogeneous catalysts for CO2 reduction, this mini-review is focused on heme and nonheme metal complexes that act as effective catalysts for the electrocatalytic and photocatalytic reduction of CO2. Because metalloporphyrinoids show strong absorption in the visible region, which is sensitive to the oxidation states of the metals and ligands, they are suited for the detection of reactive intermediates in the catalytic CO2 reduction cycle by electronic absorption spectroscopy. The first part of this review deals with the catalytic mechanism for the one-electron reduction of CO2 to oxalic acid with heme and nonheme metal complexes, with an emphasis on how the formation of highly energetic CO2˙ is avoided. Then, the catalytic mechanism of two-electron reduction of CO2 to produce CO and H2O is compared with that to produce HCOOH. The effect of metals and ligands of the heme and nonheme complexes on the CO or HCOOH product selectivity is also discussed. The catalytic mechanisms of multi-electron reduction of CO2 to methanol (six-electron reduced product) and methane (eight-electron reduced product) are also discussed for both electrocatalytic and photocatalytic systems.

Graphical abstract: Mechanisms of catalytic reduction of CO2 with heme and nonheme metal complexes

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Publication details

The article was received on 19 May 2018, accepted on 26 Jun 2018 and first published on 02 Jul 2018


Article type: Minireview
DOI: 10.1039/C8SC02220H
Chem. Sci., 2018,9, 6017-6034
  • Open access: Creative Commons BY-NC license
    All publication charges for this article have been paid for by the Royal Society of Chemistry

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    Mechanisms of catalytic reduction of CO2 with heme and nonheme metal complexes

    S. Fukuzumi, Y. Lee, H. S. Ahn and W. Nam, Chem. Sci., 2018, 9, 6017
    DOI: 10.1039/C8SC02220H

    This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material and it is not used for commercial purposes.

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