Formic acid as H2 storage system: hydrogenation of CO2 and decomposition of formic acid by solid molecular phosphine catalysts

被引：5

作者：

Kipshagen, Anna ^{[1
]}

Baums, Janine C. ^{[1
]}

Hartmann, Heinrich ^{[2
]}

Besmehn, Astrid ^{[2
]}

Hausoul, Peter J. C. ^{[1
]}

Palkovits, Regina ^{[1
,3
]}

机构：

[1] Rhein Westfal TH Aachen, Inst Tech & Makromol Chem, Worringerweg 2, D-52074 Aachen, Germany

[2] Forschungszentrum Julich, Zentralinst Engn Elekt & Analyt Analyt ZEA 3, D-52425 Julich, Germany

[3] Max Planck Inst Chem Energy Convers, Stiftstr 34-36, D-45470 Mulheim, Germany

来源：

CATALYSIS SCIENCE & TECHNOLOGY | 2022年 / 12卷 / 18期

关键词：

CARBON-DIOXIDE; HOMOGENEOUS HYDROGENATION; ROOM-TEMPERATURE; AQUEOUS-SOLUTION; RUTHENIUM; GENERATION; COMPLEXES; FORMATE; WATER; BICARBONATE;

D O I：

10.1039/d2cy00608a

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：

The synthesis and decomposition of formic acid (FA) in aqueous triethylamine (NEt3) with solid molecular phosphine catalysts is demonstrated. A Ru-catalyst based on the polymeric analog of 1,2-bis(diphenylphosphino)ethane presented the highest activity with a TON of 9680 under mild reaction conditions. Reaction parameters such as solvent, amine, pressure, time and temperature were systematically investigated. The application as a H-2 storage system was demonstrated by coupling both reactions. In recycling experiments, a decrease of the hydrogenation activity was observed, while the decomposition rate remained constant. Characterization of the spent catalyts revealed the formation of carbonyl complexes which are responsible for the observed activity difference.

引用

页码：5649 / 5656

页数：8

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