Additive-Free Ruthenium-Catalyzed Hydrogen Production from Aqueous Formaldehyde with High Efficiency and Selectivity

被引：38
|
作者：
Wang, Lin [1 ]
Ertem, Mehmed Z. [2 ]
Kanega, Ryoichi [1 ]
Murata, Kazuhisa [1 ]
Szalda, David J. [3 ]
Muckerman, James T. [2 ]
Fujita, Etsuko [2 ]
Himeda, Yuichiro [1 ]
机构：
[1] Natl Inst Adv Ind Sci & Technol, Environm & Energy Dept, Res Inst Energy Frontier, Tsukuba Cent 5,1-1-1 Higashi, Tsukuba, Ibaraki 3058565, Japan
[2] Brookhaven Natl Lab, Div Chem, Upton, NY 11973 USA
[3] CUNY, Baruch Coll, Dept Nat Sci, New York, NY 10010 USA
来源：
ACS CATALYSIS | 2018年 / 8卷 / 09期
关键词：
dehydrogenation; formaldehyde; homogeneous catalysis; ruthenium complex; H-2; production; FORMIC-ACID; CO2; HYDROGENATION; METHANOL DEHYDROGENATION; HOMOGENEOUS CATALYSTS; CARBON-DIOXIDE; WATER; COMPLEX; ENERGY; LIGAND; PARAFORMALDEHYDE;
D O I：
10.1021/acscatal.8b02088
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：
An efficient water-soluble ruthenium complex was developed for selective hydrogen production from aqueous formaldehyde under mild conditions with a high yield (similar to 95%). Hydrogen production by this catalytic system proceeds without using any additives or organic solvents, leading to a high turnover frequency (8300 h(-1)) and a record turnover number of 24 000. Moreover, based on mechanistic experiments and density functional theory (DFT) calculations, a step-by-step mechanism has been proposed for the catalytic cycle.
引用
收藏
页码：8600 / 8605
页数：11
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