CO2 Hydrogenation Catalysts with Deprotonated Picolinamide Ligands

被引：70
|
作者：
Kanega, Ryoichi [1 ]
Onishi, Naoya [1 ]
Szalda, David J. [2 ]
Ertem, Mehmed Z. [3 ]
Muckerman, James T. [3 ]
Fujita, Etsuko [3 ]
Himeda, Yuichiro [1 ]
机构：
[1] Natl Inst Adv Ind Sci & Technol, Dept Energy & Environm, Res Inst Energy Frontier, Tsukuba Cent 5,1-1-1 Higashi, Tsukuba, Ibaraki 3058565, Japan
[2] CUNY, Baruch Coll, Dept Nat Sci, New York, NY 10010 USA
[3] Brookhaven Natl Lab, Chem Div, Upton, NY 11973 USA
来源：
ACS CATALYSIS | 2017年 / 7卷 / 10期
关键词：
CO2; hydrogenation; deprotonated picolinamide ligand; water-soluble Ir catalysts; formate production; DFT calculations; hydrogen storage; CARBON-DIOXIDE; FORMIC-ACID; DENSITY FUNCTIONALS; AMBIENT-TEMPERATURE; MILD TEMPERATURES; COMPLEXES; REDUCTION; PRESSURE; IRIDIUM; STORAGE;
D O I：
10.1021/acscatal.7b02280
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
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.
引用
收藏
页码：6426 / 6429
页数：4
相关论文
共 50 条
  • [1] CO2 hydrogenation for hydrogen storage using iridium catalysts with deprotonated picolinamide ligands
    Himeda, Yuichiro
    Kanega, Ryoichi
    Onishi, Naoya
    Wang, Lin
    Ertem, Mehmed
    Muckerman, James
    Fujita, Etsuko
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2018, 256
  • [2] Efficient Cp*Ir Catalysts with Imidazoline Ligands for CO2 Hydrogenation
    Xu, Shaoan
    Onishi, Naoya
    Tsurusaki, Akihiro
    Manaka, Yuichi
    Wang, Wan-Hui
    Muckerman, James T.
    Fujita, Etsuko
    Himeda, Yuichiro
    EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2015, (34) : 5591 - 5594
  • [3] HYDROGENATION OF CO AND CO2 ON OXIDE CATALYSTS
    WILLCOX, D
    KUNG, HH
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 1985, 189 (APR-): : 14 - COLL
  • [4] Development of bifunctional catalysts containing hydride-relay ligands for CO2 hydrogenation
    Devi, Nilakshi
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2018, 255
  • [5] Design of catalysts for selective CO2 hydrogenation
    Runping Ye
    Jie Ding
    Tomas Ramirez Reina
    Melis Seher Duyar
    Haitao Li
    Wenhao Luo
    Rongbin Zhang
    Maohong Fan
    Gang Feng
    Jian Sun
    Jian Liu
    Nature Synthesis, 2025, 4 (3): : 288 - 302
  • [6] CO2 HYDROGENATION OVER CARBIDE CATALYSTS
    DUBOIS, JL
    SAYAMA, K
    ARAKAWA, H
    CHEMISTRY LETTERS, 1992, (01) : 5 - 8
  • [7] Design of catalysts for selective CO2 hydrogenation
    Ye, Runping
    Ding, Jie
    Reina, Tomas Ramirez
    Duyar, Melis Seher
    Li, Haitao
    Luo, Wenhao
    Zhang, Rongbin
    Fan, Maohong
    Feng, Gang
    Sun, Jian
    Liu, Jian
    NATURE SYNTHESIS, 2025,
  • [8] Design of catalysts for selective CO2 hydrogenation
    Ye, Runping
    Ding, Jie
    Reina, Tomas Ramirez
    Duyar, Melis Seher
    Li, Haitao
    Luo, Wenhao
    Zhang, Rongbin
    Fan, Maohong
    Feng, Gang
    Sun, Jian
    Liu, Jian
    NATURE SYNTHESIS, 2025, 4 (03): : 288 - 302
  • [9] CO2 hydrogenation to methanol by organometallic catalysts
    Onishi, Naoya
    Himeda, Yuichiro
    CHEM CATALYSIS, 2022, 2 (02): : 242 - 252
  • [10] Supported iron catalysts for CO2 hydrogenation
    Wang, Hongwang
    Shrestha, Tej
    Thapa, Prem
    Moore, David
    Hodgson, Jim
    Xu, Feng
    Wang, Donghai
    Troyer, Deryl L.
    Bossmann, Stefan H.
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2014, 247
12345