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Magnus Haugaard Rønne

Ligand-Controlled Product Selectivity in Electrochemical Carbon Dioxide Reduction Using Manganese Bipyridine Catalysts

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Ligand-Controlled Product Selectivity in Electrochemical Carbon Dioxide Reduction Using Manganese Bipyridine Catalysts. / Rønne, Magnus H.; Cho, Dasol; Madsen, Monica R.; Jakobsen, Joakim B.; Eom, Seunghwan; Escoudé, Émile; Hammershøj, Hans Christian D.; Nielsen, Dennis U.; Pedersen, Steen U.; Baik, Mu Hyun; Skrydstrup, Troels; Daasbjerg, Kim.

I: Journal of the American Chemical Society, Bind 142, Nr. 9, 03.2020, s. 4265-4275.

Publikation: Bidrag til tidsskrift/Konferencebidrag i tidsskrift /Bidrag til avisTidsskriftartikelForskningpeer review

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Author

Rønne, Magnus H. ; Cho, Dasol ; Madsen, Monica R. ; Jakobsen, Joakim B. ; Eom, Seunghwan ; Escoudé, Émile ; Hammershøj, Hans Christian D. ; Nielsen, Dennis U. ; Pedersen, Steen U. ; Baik, Mu Hyun ; Skrydstrup, Troels ; Daasbjerg, Kim. / Ligand-Controlled Product Selectivity in Electrochemical Carbon Dioxide Reduction Using Manganese Bipyridine Catalysts. I: Journal of the American Chemical Society. 2020 ; Bind 142, Nr. 9. s. 4265-4275.

Bibtex

@article{7be8178a15d440a59054dba36b2a01d7,
title = "Ligand-Controlled Product Selectivity in Electrochemical Carbon Dioxide Reduction Using Manganese Bipyridine Catalysts",
abstract = "Electrocatalysis is a promising tool for utilizing carbon dioxide as a feedstock in the chemical industry. However, controlling the selectivity for different CO2 reduction products remains a major challenge. We report a series of manganese carbonyl complexes with elaborated bipyridine or phenanthroline ligands that can reduce CO2 to either formic acid, if the ligand structure contains strategically positioned tertiary amines, or CO, if the amine groups are absent in the ligand or are placed far from the metal center. The amine-modified complexes are benchmarked to be among the most active catalysts for reducing CO2 to formic acid, with a maximum turnover frequency of up to 5500 s-1 at an overpotential of 630 mV. The conversion even works at overpotentials as low as 300 mV, although through an alternative mechanism. Mechanistically, the formation of a Mn-hydride species aided by in situ protonated amine groups was determined to be a key intermediate by cyclic voltammetry, 1H NMR, DFT calculations, and infrared spectroelectrochemistry.",
keywords = "COMPLEXES, CYCLIC VOLTAMMETRY, ELECTROCATALYTIC CO2 REDUCTION, ELECTRON-TRANSFER, ELECTROREDUCTION, FORMATE, LOCAL PROTON SOURCE, MOLECULAR CATALYSIS, RHENIUM, WEAK BRONSTED ACIDS",
author = "R{\o}nne, {Magnus H.} and Dasol Cho and Madsen, {Monica R.} and Jakobsen, {Joakim B.} and Seunghwan Eom and {\'E}mile Escoud{\'e} and Hammersh{\o}j, {Hans Christian D.} and Nielsen, {Dennis U.} and Pedersen, {Steen U.} and Baik, {Mu Hyun} and Troels Skrydstrup and Kim Daasbjerg",
year = "2020",
month = mar,
doi = "10.1021/jacs.9b11806",
language = "English",
volume = "142",
pages = "4265--4275",
journal = "Journal of the American Chemical Society",
issn = "0002-7863",
publisher = "ACS Publications",
number = "9",

}

RIS

TY - JOUR

T1 - Ligand-Controlled Product Selectivity in Electrochemical Carbon Dioxide Reduction Using Manganese Bipyridine Catalysts

AU - Rønne, Magnus H.

AU - Cho, Dasol

AU - Madsen, Monica R.

AU - Jakobsen, Joakim B.

AU - Eom, Seunghwan

AU - Escoudé, Émile

AU - Hammershøj, Hans Christian D.

AU - Nielsen, Dennis U.

AU - Pedersen, Steen U.

AU - Baik, Mu Hyun

AU - Skrydstrup, Troels

AU - Daasbjerg, Kim

PY - 2020/3

Y1 - 2020/3

N2 - Electrocatalysis is a promising tool for utilizing carbon dioxide as a feedstock in the chemical industry. However, controlling the selectivity for different CO2 reduction products remains a major challenge. We report a series of manganese carbonyl complexes with elaborated bipyridine or phenanthroline ligands that can reduce CO2 to either formic acid, if the ligand structure contains strategically positioned tertiary amines, or CO, if the amine groups are absent in the ligand or are placed far from the metal center. The amine-modified complexes are benchmarked to be among the most active catalysts for reducing CO2 to formic acid, with a maximum turnover frequency of up to 5500 s-1 at an overpotential of 630 mV. The conversion even works at overpotentials as low as 300 mV, although through an alternative mechanism. Mechanistically, the formation of a Mn-hydride species aided by in situ protonated amine groups was determined to be a key intermediate by cyclic voltammetry, 1H NMR, DFT calculations, and infrared spectroelectrochemistry.

AB - Electrocatalysis is a promising tool for utilizing carbon dioxide as a feedstock in the chemical industry. However, controlling the selectivity for different CO2 reduction products remains a major challenge. We report a series of manganese carbonyl complexes with elaborated bipyridine or phenanthroline ligands that can reduce CO2 to either formic acid, if the ligand structure contains strategically positioned tertiary amines, or CO, if the amine groups are absent in the ligand or are placed far from the metal center. The amine-modified complexes are benchmarked to be among the most active catalysts for reducing CO2 to formic acid, with a maximum turnover frequency of up to 5500 s-1 at an overpotential of 630 mV. The conversion even works at overpotentials as low as 300 mV, although through an alternative mechanism. Mechanistically, the formation of a Mn-hydride species aided by in situ protonated amine groups was determined to be a key intermediate by cyclic voltammetry, 1H NMR, DFT calculations, and infrared spectroelectrochemistry.

KW - COMPLEXES

KW - CYCLIC VOLTAMMETRY

KW - ELECTROCATALYTIC CO2 REDUCTION

KW - ELECTRON-TRANSFER

KW - ELECTROREDUCTION

KW - FORMATE

KW - LOCAL PROTON SOURCE

KW - MOLECULAR CATALYSIS

KW - RHENIUM

KW - WEAK BRONSTED ACIDS

UR - http://www.scopus.com/inward/record.url?scp=85080120357&partnerID=8YFLogxK

U2 - 10.1021/jacs.9b11806

DO - 10.1021/jacs.9b11806

M3 - Journal article

C2 - 32022558

AN - SCOPUS:85080120357

VL - 142

SP - 4265

EP - 4275

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 9

ER -