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Title: CO 2 Hydrogenation Catalysts with Deprotonated Picolinamide Ligands

In an effort to design concepts for highly active catalysts for the hydrogenation of CO 2 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 CO 2 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] ; ORCiD logo [1] ;  [2] ;  [3] ;  [3] ; ORCiD logo [3] ; ORCiD logo [1]
  1. National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
  2. Baruch College, New York, NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Report Number(s):
BNL-114356-2017-JA
Journal ID: ISSN 2155-5435; R&D Project: CO026; KC0304030
Grant/Contract Number:
SC0012704; JPMJCR12Z0
Type:
Published Article
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 7; Journal Issue: 10; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States); National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Japan Science and Technology Agency (JST)
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
OSTI Identifier:
1377083
Alternate Identifier(s):
OSTI ID: 1395940

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., 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. doi:10.1021/acscatal.7b02280.
Kanega, Ryoichi, Onishi, Naoya, Szalda, David J., Ertem, Mehmed Z., Muckerman, James T., Fujita, Etsuko, and Himeda, Yuichiro. 2017. "CO2 Hydrogenation Catalysts with Deprotonated Picolinamide Ligands". United States. doi: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 = 10,
volume = 7,
place = {United States},
year = {2017},
month = {8}
}