Polymers are used in simple consumer items like carpets, furniture, glues, and clothing but are also used in advanced engineering, including materials used in the aerospace industry. Therefore, pol...

Catalytic Approaches to Monomers for Polymers Based on Renewables

A series of Cu/dolomite catalysts were synthesized using the impregnation technique, characterized using NH3–TPD, FTIR-Pyridine, XRD, H2-TPR, BET, BJH, FESEM-EDX, and XPS techniques and evaluated in glycerol hydrogenolysis into 1,2-propanediol (1,2-PDO). Remarkably, dolomite support exhibited high acidity, which is, to our knowledge the first acid characteristic revealed among the reported literatures. By doping copper on dolomite support, the acid amount and strength of the catalyst increased. N2O chemisorption analysis suggests that the metallic copper species were well dispersed on dolomite support while the copper surface area increased with copper loading. The formation of metallic copper on dolomite support agreed well with findings derived from XRD and XPS analysis. According to the results of XPS and H2-TPR, metallic copper species were enriched on the grain surfaces of dolomite and not in the bulk. The addition of copper to dolomite ameliorates the redox properties of the catalysts, owing to the reduction at a lower temperature than that of pure CuO and dolomite support. From the catalytic results, 20 wt% Cu/dolomite was the most active catalyst by giving 100% glycerol conversion and 92% selectivity toward 1,2-PDO at 180 oC, 2 MPa H2 in 6 h reaction time.

Copper-dolomite as effective catalyst for glycerol hydrogenolysis to 1,2-propanediol

A kinetic study on the liquid phase hydrogenolysis of glycerol was carried out in a slurry reactor in the presence of a highly selective Cu–Ni–Al2O3 catalyst at different reaction temperatures (180–220 °C) and pressures (3–6 MPa), and very high selectivity was achieved (∼95%) towards 1,2-propanediol (1,2-PDO). A series of reaction schemes for the conversion of glycerol to 1,2-PDO followed by the hydrogenolysis of 1,2-PDO to propanol was considered to develop the kinetic model. Initially, the power-law model was fitted followed by a modified power-law model considering 1,2-PDO and propanol (1-PO + 2-PO) as the main reaction products. To understand the intrinsic kinetic behaviour, a more realistic heterogeneous kinetic model based on a combined Langmuir–Hinshelwood–Hougen–Watson (LHHW) and Eley–Rideal (ER) approach was developed. The numerical solution for the model equation was computed using ode23 solver in MATLAB combined with the genetic algorithm. The results demonstrated that the experimental concentrations were well-fitted with the model-predicted concentration. The calculated activation energy was 70.5 kJ mol−1 for the conversion of glycerol to 1,2-PDO and 79.5 kJ mol−1 for the production of PO from 1,2-PDO. The parity plots of the experimental and model simulated concentration of the reactant and products were fitted very well.

Kinetic modelling for the hydrogenolysis of bio-glycerol in the presence of a highly selective Cu–Ni–Al2O3 catalyst in a slurry reactor

A highly efficient Cu/AlOOH catalyst obtained by in situ reduction: Catalytic transfer hydrogenation of ML into γ-GVL

Selective hydrogenolysis of bioglycerol to 1,3-propanedilo (1,3-PDO) is regarded as a perfect combination of a valorization of biomass-derived glycerol and an increasing demand for 1,3-propanediol. In this work, SiO2 gel was impregnated by Al(NO3)3·9H2O followed by a calcination at a high temperature, and a strong interaction between SiO2 and Al2O3 led to a homogeneous dispersion of the Al2O3 on the surface of the substrate SiO2. The Al2O3-decorated SiO2 was used to load WOx and Pt sequentially and the resulting Pt–WOx/SiO2–Al2O3 catalysts were found a markedly enhanced surface acidity due to a strong interaction between the Al2O3-modified support and the WOx domain as well as the introduced ion exchange functionality by Al2O3 addition. A well-defined matching between the acidic and metallic sites was realized by turning the content of the Al2O3, and the glycerol conversion and 1,3-PDO selectivity were enhanced by a large margin on the optimized Pt–WOx/SiO2–Al2O3 catalyst. A markedly improved reactivity in bioglycerol hydrogenolysis was realized using the Pt–WOx catalysts supported over Al2O3-modified SiO2.

Promotion Effect of Al2O3 on Pt–WOx/SiO2 Catalysts for Selective Hydrogenolysis of Bioglycerol to 1,3-Propanediol in Liquid Phase

Activity improvement of Ru-based catalysts is needed for efficient production of valuable chemicals from glycerol hydrogenolysis. In this work, a series of Re promoted Ru catalysts encapuslated in porous silica nanoparticles (denoted as Re-Ru@SiO2) were prepared by coating silica onto the surface of chemically reduced Ru-polyvinylpyrrolidone colloids, and were used to catalyze the conversion of glycerol to diols and alcohols in water. X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), nitrogen adsorption, X-ray photoelectron spectroscopy (XPS) and temperature-programmed reduction (TPR) were used to characterize these nanoparticles. Effects of Ru/Si atomic ratio, Re addition, glycerol and catalyst concentrations, reaction time, temperature, and hydrogen pressure were investigated. Re addition retarded the reduction of ruthenium oxide, but increased the catalyst reactivity for glycerol hydrogenolysis. Due to its greater Ru content, Re-Ru@ SiO2 showed much better activity (reacted at much lower temperature) and more yields of 1,2-propanediol and overall liquid-phase products than Re-Ru/SiO2 (prepared by conventional impregnation method) reported before. The rate of glycerol disappearance exhibited first-order dependence on glycerol concentration and hydrogen pressure, with an activation energy of 107.8 kJ/mol. The rate constant increased linearly with increasing Ru/Si atomic ratio and catalyst amount. The yield of overall liquid-phase products correlated well with glycerol conversion.

Aqueous-Phase Hydrogenolysis of Glycerol over Re Promoted Ru Catalysts Encapuslated in Porous Silica Nanoparticles.

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Aqueous-Phase Hydrogenolysis of Glycerol over Re Promoted Ru Catalysts Encapuslated in Porous Silica Nanoparticles.