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Heterogeneous Silica‐Supported Ruthenium Phosphine Catalysts for Selective Formic Acid Decomposition
Author(s) -
Gan Weijia,
Dyson Paul J.,
Laurenczy Gábor
Publication year - 2013
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.201300246
Subject(s) - tppts , ruthenium , catalysis , formic acid , chemistry , phosphine , triphenylphosphine , diphenylphosphine , aqueous solution , leaching (pedology) , inorganic chemistry , nuclear chemistry , organic chemistry , rhodium , hydroformylation , environmental science , soil science , soil water
The water‐soluble ruthenium(II)– m TPPTS complex ( m TPPTS= meta ‐trisulfonated triphenylphosphine) efficiently catalyzes the generation of hydrogen from formic acid in aqueous solution. This catalyst has been immobilized in a hydrophilic silica support to facilitate mobile portable applications. It was used in diluted formic acid solutions, in which the recycling of a liquid phase catalyst is problematic. A series of heterogenized catalysts have been prepared by the reaction of the ruthenium(II)– m TPPTS dimer and silica functionalized with diphenylphosphine groups via alkyl chains. The length of the alkylene chain separating the silica from the diphenylphosphine group has been varied in these catalysts—all of them catalyzing the decomposition of formic acid. The catalysts were easily separated from the solution and reused. The optimized catalytic system based on MCM41‐Si‐(CH 2 ) 2 PPh 2 /Ru‐ m TPPTS demonstrated an activity and stability comparable to those of the homogeneous catalyst: a turnover frequency of 2780 h −1 was obtained at 110 °C, and no ruthenium leaching was detected after turnover numbers of 71 000.