Zirconium-based Metal Composite Materials For The Catalytic Transfer Hydrogenation Of Biomass-derived Compounds

With the surge in the population of the world and the sharp increase in the demand for non-renewable fossil fuels,humans are facing an energy crisis.Researchers are eager to develop environmentally friendly and renewable energy to achieve sustainable development.As an alternative,biomass is an inexhaustible,cheap,and environmentally friendly natural resources.Therefore,biomass hydrogenation is especially important for biofuels.Conventional hydrogenation used hydrogen as a hydrogen source,which is neither environmental conservation nor safe.So researchers have developed green sustainable and more convenient use of alcohol-based catalytic transfer hydrogenation systems to reduce biomass-derived carbonyl compounds to high value additions.This thesis is committed to developing low cost,high efficient,high stable catalyst,applying to the hydrogenation of FAL and LA.The content of this thesis is as follows:1.A magnetic zirconium hydroxide catalyst is designed for a catalytic transfer hydrogenation reaction for biomass derived carbonyl compounds.The catalyst composites zirconium hydroxide with ferric acid to prepare a synthesis of simple,simply simple magnetic nuclear shell material,and exhibits high catalytic activity,especially in a reaction of furfural hydrogenation into a furfuryl alcohol.The catalyst,at a suitable temperature(160 °C),reached 93.9 % furfural conversion and 97.3 % of furfuryl alcohol selectivity,which is at a very high level in reported magnetic material.At the same time,we also test the catalyst for recycling.It was found that it can reach91.1% furfural conversion and 97.8% of the furfuryl alcohol selectivity after 7 cycles.The structural stability of the catalyst was demonstrated by infrared spectroscopy,elemental analysis and thermogravimetric analysis.Then we have expanded the scale of the reaction to ten times and obtain the results similar to the conventional catalytic reaction,which proves the potential of the catalyst has industrial production.2.A metal-doped carbon material was synthesized by a one-pot method of zirconium salt and glucose and applied to the catalytic transfer hydrogenation of levulinic acid(LA)to produce γ-valerolactone(GVL).The catalyst was designed from the side reaction that occurs during the catalytic reaction.Adjusting different ratios of metal and glucose,we found that the best catalytic effect was achieved at a ratio of 4:1,reaching 91.5% LA conversion and 95.2% GVL selectivity.It was also found that different feeding ratios of Zr and glucose showed regular results.The conversion of LA increases with Zr doping and the resulting side reaction decreases with the increase of glucose.Then we studied the route of the reaction and the origin of the products by changing the experimental conditions.Finally,based on the experimental results and previous reports,a possible reaction mechanism and the approximate structure of Humins were proposed.