4.8 Article

CO2 Hydrogenation Catalysts with Deprotonated Picolinamide Ligands

期刊

ACS CATALYSIS
卷 7, 期 10, 页码 6426-6429

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b02280

关键词

CO2 hydrogenation; deprotonated picolinamide ligand; water-soluble Ir catalysts; formate production; DFT calculations; hydrogen storage

资金

  1. JST ACT-C, Japan [JPMJCR12Z0]
  2. U.S. Department of Energy, Office of Science, Division of Chemical Sciences, Geosciences & Biosciences, Office of Basic Energy Sciences [DE-SC0012704]

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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-methylpicolinamidate ligand exhibited excellent activity even under ambient conditions (0.1 MPa, 25 degrees 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.

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