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

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页码：8600 / 8605

页数：11

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