Mechanistic aspects of CO2 reduction catalysis with manganese-based molecular catalysts

David Grills, Mehmed Z. Ertem, Meaghan McKinnon, Ken T. Ngo, Jonathan Rochford

Research output: Contribution to journalReview article

12 Citations (Scopus)

Abstract

One approach for the conversion of CO2 into fuels or fuel precursors is the proton-coupled reduction of CO2 to CO or formic acid, using transition metal complexes as catalysts in either electrocatalytic or photocatalytic processes. While a number of such molecular catalysts have been investigated over the years, many are based on expensive precious metals. However, a growing family of pre-catalysts based on the earth-abundant metal, manganese, originally with the generic formula, [Mn(α-diimine)(CO)3L]+/0, but now expanded to also include non-α-diimine ligands, has recently emerged as a promising, cheaper alternative to the heavily-investigated rhenium-based analogues. In this review, we discuss the current mechanistic understanding of Mn-based CO2 reduction pre-catalysts, from the point of view of both computational modeling and experimental techniques. We also highlight the methods used to accurately determine catalytic figures of merit, such as overpotential and turnover frequency. Finally, we have summarized the major findings in both electrocatalytic and photocatalytic CO2 reduction driven by Mn-based catalysts, including exciting new developments involving immobilization of the molecular catalysts on solid supports or electrodes, and also their use in photoelectrochemical CO2 reduction where solar energy is used to overcome the demanding electrochemical overpotential.

Original languageEnglish
Pages (from-to)173-217
Number of pages45
JournalCoordination Chemistry Reviews
Volume374
DOIs
Publication statusPublished - Nov 1 2018

Fingerprint

Manganese
Catalysis
catalysis
manganese
catalysts
Catalysts
formic acid
Carbon Monoxide
Rhenium
Formic acid
Coordination Complexes
rhenium
solar energy
Precious metals
Metal complexes
noble metals
immobilization
Catalyst supports
figure of merit
Solar energy

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

Mechanistic aspects of CO2 reduction catalysis with manganese-based molecular catalysts. / Grills, David; Ertem, Mehmed Z.; McKinnon, Meaghan; Ngo, Ken T.; Rochford, Jonathan.

In: Coordination Chemistry Reviews, Vol. 374, 01.11.2018, p. 173-217.

Research output: Contribution to journalReview article

Grills, David ; Ertem, Mehmed Z. ; McKinnon, Meaghan ; Ngo, Ken T. ; Rochford, Jonathan. / Mechanistic aspects of CO2 reduction catalysis with manganese-based molecular catalysts. In: Coordination Chemistry Reviews. 2018 ; Vol. 374. pp. 173-217.
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