CO2 Hydrogenation Catalysts with Deprotonated Picolinamide Ligands
Abstract
In an effort to design concepts for highly active catalysts for the hydrogenation of CO2 to formate in basic water, we have prepared in this paper several catalysts with picolinic acid, picolinamide, and its derivatives, and we investigated their catalytic activity. The CO2 hydrogenation catalyst having a 4-hydroxy-N-methylpicolinamidate ligand exhibited excellent activity even under ambient conditions (0.1 MPa, 25 °C) in basic water, exhibiting a TON of 14700, a TOF of 167 h–1, and producing a 0.64 M formate concentration. Finally, its high catalytic activity originates from strong electron donation by the anionic amide moiety in addition to the phenolic O– functionality.
- Authors:
-
[1];
[3];
[1]
- Research Institute of Energy Frontier, Department of Energy and Environment, National Institute of Advanced Industrial Science and Technology, Tsukuba Central 5, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan
- Department of Natural Science, Baruch College, CUNY, New York, New York 10010-5585, United States
- Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973-5000, United States
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States); National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
- Sponsoring Org.:
- Japan Science and Technology Agency (JST); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1377083
- Alternate Identifier(s):
- OSTI ID: 1395940; OSTI ID: 1507720
- Report Number(s):
- BNL-114356-2017-JA
Journal ID: ISSN 2155-5435
- Grant/Contract Number:
- SC0012704; JPMJCR12Z0
- Resource Type:
- Published Article
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Name: ACS Catalysis; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 hydrogenation; deprotonated picolinamide ligand; DFT calculations; formate production; hydrogen storage; water-soluble Ir catalysts
Citation Formats
Kanega, Ryoichi, Onishi, Naoya, Szalda, David J., Ertem, Mehmed Z., Muckerman, James T., Fujita, Etsuko, and Himeda, Yuichiro. CO2 Hydrogenation Catalysts with Deprotonated Picolinamide Ligands. United States: N. p., 2017.
Web. doi:10.1021/acscatal.7b02280.
Kanega, Ryoichi, Onishi, Naoya, Szalda, David J., Ertem, Mehmed Z., Muckerman, James T., Fujita, Etsuko, & Himeda, Yuichiro. CO2 Hydrogenation Catalysts with Deprotonated Picolinamide Ligands. United States. https://doi.org/10.1021/acscatal.7b02280
Kanega, Ryoichi, Onishi, Naoya, Szalda, David J., Ertem, Mehmed Z., Muckerman, James T., Fujita, Etsuko, and Himeda, Yuichiro. Fri .
"CO2 Hydrogenation Catalysts with Deprotonated Picolinamide Ligands". United States. https://doi.org/10.1021/acscatal.7b02280.
@article{osti_1377083,
title = {CO2 Hydrogenation Catalysts with Deprotonated Picolinamide Ligands},
author = {Kanega, Ryoichi and Onishi, Naoya and Szalda, David J. and Ertem, Mehmed Z. and Muckerman, James T. and Fujita, Etsuko and Himeda, Yuichiro},
abstractNote = {In an effort to design concepts for highly active catalysts for the hydrogenation of CO2 to formate in basic water, we have prepared in this paper several catalysts with picolinic acid, picolinamide, and its derivatives, and we investigated their catalytic activity. The CO2 hydrogenation catalyst having a 4-hydroxy-N-methylpicolinamidate ligand exhibited excellent activity even under ambient conditions (0.1 MPa, 25 °C) in basic water, exhibiting a TON of 14700, a TOF of 167 h–1, and producing a 0.64 M formate concentration. Finally, its high catalytic activity originates from strong electron donation by the anionic amide moiety in addition to the phenolic O– functionality.},
doi = {10.1021/acscatal.7b02280},
journal = {ACS Catalysis},
number = ,
volume = ,
place = {United States},
year = {Fri Aug 25 00:00:00 EDT 2017},
month = {Fri Aug 25 00:00:00 EDT 2017}
}
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https://doi.org/10.1021/acscatal.7b02280
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Cited by: 54 works
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Figures / Tables:
Scheme 1: Mononuclear Catalysts for Selective CO2 Hydrogenation to Generate Formate under Ambient Conditions in Basic Water (pH ∼ 8.2)
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