Highly Efficient Reversible Hydrogenation of Carbon Dioxide to Formates Using a Ruthenium PNP-Pincer Catalyst

The use of hydrogen as a fuel requires both safe and robust technologies for its storage and transportation. Formic acid (FA) produced by the catalytic hydrogenation of CO2 is recognized as a potential intermediate H2 carrier. Herein, we present the development of a formate‐based H2 storage system t...

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Vydáno v:ChemCatChem Ročník 6; číslo 6; s. 1526 - 1530
Hlavní autoři: Filonenko, Georgy A., van Putten, Robbert, Schulpen, Erik N., Hensen, Emiel J. M., Pidko, Evgeny A.
Médium: Journal Article
Jazyk:angličtina
Vydáno: Weinheim WILEY-VCH Verlag 01.06.2014
WILEY‐VCH Verlag
Wiley Subscription Services, Inc
Témata:
Carbon dioxide
homogeneous catalysis
hydrogen
hydrogenation
reaction mechanisms
ruthenium
ISSN:1867-3880, 1867-3899
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Shrnutí:The use of hydrogen as a fuel requires both safe and robust technologies for its storage and transportation. Formic acid (FA) produced by the catalytic hydrogenation of CO2 is recognized as a potential intermediate H2 carrier. Herein, we present the development of a formate‐based H2 storage system that employs a Ru PNP‐pincer catalyst. The high stability of this system allows cyclic operation with an exceptionally fast loading and liberation of H2. Kinetic studies highlight the crucial role of the base promoter, which controls the rate‐determining step in FA dehydrogenation and defines the total H2 capacity attainable from the hydrogenation of CO2. The reported findings show promise for the development of practical technologies that use formic acid as a hydrogen carrier. Like pinning down an ant: An Ru PNP catalyst provides unprecedented rates of CO2 hydrogenation up to 1 100 000 h−1 (turnover number >200 000) and excellent activity in the dehydrogenation of formic acid in DMF if used with the non‐nucleophilic 1,8‐diazabicyclo[5.4.0]undec‐7‐ene base. Unlike amine‐based systems, this medium allows us to achieve high formate capacity together with rapid H2 charging and release.
Bibliografie:ark:/67375/WNG-9S9GDVVJ-0
ArticleID:CCTC201402119
Technology Foundation STW
Netherlands Organization for Scientific Research (NWO)
istex:B76054ED6BB3841C331D0BA4805BB4EDF9EC56FF
ObjectType-Article-1
SourceType-Scholarly Journals-1
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ISSN:1867-3880
1867-3899
DOI:10.1002/cctc.201402119