Novel aqueous-phase hydrogenation reaction of the key biorefinery platform chemical levulinic acid into γ-valerolactone employing highly active, selective and stable water-soluble ruthenium catalysts modified with nitrogen-containing ligands

被引:39
|
作者
Moustani, Chrysavgi [1 ]
Anagnostopoulou, Eleni [1 ]
Krommyda, Kalliopi [1 ]
Panopoulou, Christina [1 ]
Koukoulakis, Konstantinos G. [2 ]
Bakeas, Evangelos B. [2 ]
Papadogianakis, Georgios [1 ]
机构
[1] Natl & Kapodistrian Univ Athens, Dept Chem, Ind Chem Lab, Athens 15771, Greece
[2] Natl & Kapodistrian Univ Athens, Dept Chem, Lab Analyt Chem, Athens 15771, Greece
关键词
Hydrogenation; Biorefinery; Levulinic acid; gamma-valerolactone; Water; METHYL-ESTERS; TRISULFONATED TRIPHENYLPHOSPHINE; HOMOGENEOUS HYDROGENATIONS; BIPHASIC HYDROGENATION; AEROBIC OXIDATION; SPECIAL-ISSUE; BIOMASS; CONVERSIONS; BIOFUELS; LIQUID;
D O I
10.1016/j.apcatb.2018.07.009
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
High catalytic activities (TOF = 3000 h(-1)) have been achieved by novel water-soluble ruthenium catalysts modified with nitrogen-containing ligands such as the bathophenanthrolinedisulfonic acid disodium salt (BPhDS) in the hydrogenation reaction of the renewable polar platform chemical levulinic acid (LA) which possesses a central relevance in the development of biorefineries of the future in a sustainable way to produce with essentially quantitative selectivity of 99.9 mol% gamma-valerolactone (GVL) in aqueous media. The apparent activation energy of the Ru/BPhDS catalyst was calculated and amounts a relative low value of 53.3 kJ/mol when one considers that in the LA h ydrogenation reaction this catalyst reduces a less reactive keto group into alcohol functionality. A recycling experiment of the Ru/BPhDS catalyst by extraction after addition of diethyl ether has shown that the catalyst is stable without loss of activity and selectivity in a consecutive run.
引用
收藏
页码:82 / 92
页数:11
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