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

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 paper, 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. In conclusion, 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.

Authors:
 [1];  [1];  [2];  [2];  [2]
+ Show Author Affiliations
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  2. Univ. of Massachusetts, Boston, MA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); University of Massachusetts, Boston, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1460701
Alternate Identifier(s):
OSTI ID: 1564413
Report Number(s):
BNL-207838-2018-JAAM
Journal ID: ISSN 0010-8545
Grant/Contract Number:  
SC0012704; CHE-1301132
Resource Type:
Accepted Manuscript
Journal Name:
Coordination Chemistry Reviews
Additional Journal Information:
Journal Volume: 374; Journal ID: ISSN 0010-8545
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Grills, David C., Ertem, Mehmed Z., McKinnon, Meaghan, Ngo, Ken T., and Rochford, Jonathan. Mechanistic aspects of CO2 reduction catalysis with manganese-based molecular catalysts. United States: N. p., 2018. Web. doi:10.1016/j.ccr.2018.05.022.
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Grills, David C., Ertem, Mehmed Z., McKinnon, Meaghan, Ngo, Ken T., & Rochford, Jonathan. Mechanistic aspects of CO2 reduction catalysis with manganese-based molecular catalysts. United States. https://doi.org/10.1016/j.ccr.2018.05.022
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Grills, David C., Ertem, Mehmed Z., McKinnon, Meaghan, Ngo, Ken T., and Rochford, Jonathan. Wed . "Mechanistic aspects of CO2 reduction catalysis with manganese-based molecular catalysts". United States. https://doi.org/10.1016/j.ccr.2018.05.022. https://www.osti.gov/servlets/purl/1460701.
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@article{osti_1460701,
title = {Mechanistic aspects of CO2 reduction catalysis with manganese-based molecular catalysts},
author = {Grills, David C. and Ertem, Mehmed Z. and McKinnon, Meaghan and Ngo, Ken T. and Rochford, Jonathan},
abstractNote = {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 paper, 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. In conclusion, 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.},
doi = {10.1016/j.ccr.2018.05.022},
journal = {Coordination Chemistry Reviews},
number = ,
volume = 374,
place = {United States},
year = {Wed Jul 18 00:00:00 EDT 2018},
month = {Wed Jul 18 00:00:00 EDT 2018}
}
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