CO2 hydrogenation catalysts with deprotonated picolinamide ligands

Ryoichi Kanega; Naoya Onishi; David J. Szalda; Mehmed Z. Ertem; James T. Muckerman; Etsuko Fujita; Yuichiro Himeda

doi:10.1021/acscatal.7b02280

CO₂ hydrogenation catalysts with deprotonated picolinamide ligands

Ryoichi Kanega, Naoya Onishi, David J. Szalda, Mehmed Z. Ertem, James T. Muckerman, Etsuko Fujita, Yuichiro Himeda

Brookhaven National Laboratory

Research output: Contribution to journal › Article

24 Citations (Scopus)

Abstract

In an effort to design concepts for highly active catalysts for the hydrogenation of CO₂ to formate in basic water, we have prepared several catalysts with picolinic acid, picolinamide, and its derivatives, and we investigated their catalytic activity. The CO₂ hydrogenation catalyst having a 4-hydroxy-N-methylpicolina-midate 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. Its high catalytic activity originates from strong electron donation by the anionic amide moiety in addition to the phenolic O^- functionality.

Original language	English
Pages (from-to)	6426-6429
Number of pages	4
Journal	ACS Catalysis
Volume	7
Issue number	10
DOIs	https://doi.org/10.1021/acscatal.7b02280
Publication status	Published - Jan 1 2017

Keywords

CO hydrogenation
DFT calculations
Deprotonated picolinamide ligand
Formate production
Hydrogen storage
Water-soluble Ir catalysts

ASJC Scopus subject areas

Catalysis
Chemistry(all)

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10.1021/acscatal.7b02280

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Kanega, R., Onishi, N., Szalda, D. J., Ertem, M. Z., Muckerman, J. T., Fujita, E., & Himeda, Y. (2017). CO₂ hydrogenation catalysts with deprotonated picolinamide ligands. ACS Catalysis, 7(10), 6426-6429. https://doi.org/10.1021/acscatal.7b02280

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abstract = "In an effort to design concepts for highly active catalysts for the hydrogenation of CO2 to formate in basic water, we have prepared several catalysts with picolinic acid, picolinamide, and its derivatives, and we investigated their catalytic activity. The CO2 hydrogenation catalyst having a 4-hydroxy-N-methylpicolina-midate 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. Its high catalytic activity originates from strong electron donation by the anionic amide moiety in addition to the phenolic O- functionality.",

keywords = "CO hydrogenation, DFT calculations, Deprotonated picolinamide ligand, Formate production, Hydrogen storage, Water-soluble Ir catalysts",

author = "Ryoichi Kanega and Naoya Onishi and Szalda, {David J.} and Ertem, {Mehmed Z.} and Muckerman, {James T.} and Etsuko Fujita and Yuichiro Himeda",

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T1 - CO2 hydrogenation catalysts with deprotonated picolinamide ligands

AU - Kanega, Ryoichi

AU - Onishi, Naoya

AU - Szalda, David J.

AU - Ertem, Mehmed Z.

AU - Muckerman, James T.

AU - Fujita, Etsuko

AU - Himeda, Yuichiro

PY - 2017/1/1

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AB - In an effort to design concepts for highly active catalysts for the hydrogenation of CO2 to formate in basic water, we have prepared several catalysts with picolinic acid, picolinamide, and its derivatives, and we investigated their catalytic activity. The CO2 hydrogenation catalyst having a 4-hydroxy-N-methylpicolina-midate 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. Its high catalytic activity originates from strong electron donation by the anionic amide moiety in addition to the phenolic O- functionality.

KW - CO hydrogenation

KW - DFT calculations

KW - Deprotonated picolinamide ligand

KW - Formate production

KW - Hydrogen storage

KW - Water-soluble Ir catalysts

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