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

页码：6426 / 6429

页数：4

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