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Title: An Investigation of Electrocatalytic CO2 Reduction Using a Manganese Tricarbonyl Biquinoline Complex

Abstract

The subject of this study [fac-Mn(bqn)(CO)3(CH3CN)]+ (bqn = 2,2'-biquinoline), is of particular interest because the bqn ligand exhibits both steric and electronic influence over the fundamental redox properties of the complex and, consequently, its related catalytic properties with respect to the activation of CO2. While not a particularly efficient catalyst for CO2 to CO conversion, in-situ generation and activity measurements of the [fac-Mn(bqn)(CO)3]- active catalyst allows for a better understanding of ligand design at the Mn center. By making direct comparisons to the related 2,2'-bipyridyl (bpy), 1,10-phenanthroline (phen), and 2,9-dimethyl-1,10-phenanthroline (dmphen) ligands via a combination of voltammetry, infrared spectroelectrochemistry, controlled potential electrolysis and computational analysis, the role of steric vs. electronic influences on the nucleophilicity of Mn-based CO2 reduction electrocatalysts is discussed.

Authors:
 [1];  [1];  [1];  [2];  [2];  [1]
  1. Univ. of Massachusetts, Boston, MA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1571410
Report Number(s):
BNL-212221-2019-JAAM
Journal ID: ISSN 2296-2646
Grant/Contract Number:  
SC0012704; CHE-1800062
Resource Type:
Accepted Manuscript
Journal Name:
Frontiers in Chemistry
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2296-2646
Publisher:
Frontiers Research Foundation
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; carbon dioxide reduction; electrocatalysis; manganese; carbon monoxide

Citation Formats

McKinnon, Meaghan, Belkina, Veronika, Ngo, Ken T., Ertem, Mehmed Z., Grills, David C., and Rochford, Jonathan. An Investigation of Electrocatalytic CO2 Reduction Using a Manganese Tricarbonyl Biquinoline Complex. United States: N. p., 2019. Web. doi:10.3389/fchem.2019.00628.
McKinnon, Meaghan, Belkina, Veronika, Ngo, Ken T., Ertem, Mehmed Z., Grills, David C., & Rochford, Jonathan. An Investigation of Electrocatalytic CO2 Reduction Using a Manganese Tricarbonyl Biquinoline Complex. United States. doi:10.3389/fchem.2019.00628.
McKinnon, Meaghan, Belkina, Veronika, Ngo, Ken T., Ertem, Mehmed Z., Grills, David C., and Rochford, Jonathan. Tue . "An Investigation of Electrocatalytic CO2 Reduction Using a Manganese Tricarbonyl Biquinoline Complex". United States. doi:10.3389/fchem.2019.00628. https://www.osti.gov/servlets/purl/1571410.
@article{osti_1571410,
title = {An Investigation of Electrocatalytic CO2 Reduction Using a Manganese Tricarbonyl Biquinoline Complex},
author = {McKinnon, Meaghan and Belkina, Veronika and Ngo, Ken T. and Ertem, Mehmed Z. and Grills, David C. and Rochford, Jonathan},
abstractNote = {The subject of this study [fac-Mn(bqn)(CO)3(CH3CN)]+ (bqn = 2,2'-biquinoline), is of particular interest because the bqn ligand exhibits both steric and electronic influence over the fundamental redox properties of the complex and, consequently, its related catalytic properties with respect to the activation of CO2. While not a particularly efficient catalyst for CO2 to CO conversion, in-situ generation and activity measurements of the [fac-Mn(bqn)(CO)3]- active catalyst allows for a better understanding of ligand design at the Mn center. By making direct comparisons to the related 2,2'-bipyridyl (bpy), 1,10-phenanthroline (phen), and 2,9-dimethyl-1,10-phenanthroline (dmphen) ligands via a combination of voltammetry, infrared spectroelectrochemistry, controlled potential electrolysis and computational analysis, the role of steric vs. electronic influences on the nucleophilicity of Mn-based CO2 reduction electrocatalysts is discussed.},
doi = {10.3389/fchem.2019.00628},
journal = {Frontiers in Chemistry},
number = ,
volume = 7,
place = {United States},
year = {2019},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Figure 1 Figure 1: Molecular structures of complexes investigated.

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