Design Of Supported Catalysts And Their Application In The Preparation Of 2-methylfuran And 3-acetylpropanol

Biomass and its derivatives play an important role in replacing fossil fuels as renewable energy.Furfural(FFA)is an important biomass-based compound that has been industrialized.The conversion of FFA to fine chemicals is an important technical means for high-value utilization of biomass.3-acetylpropanol(3-AP)is the active ingredient in synthetic drugs.Industrially,it can be obtained from 2-methylfuran(2MF),the hydrodeoxygenation product of FFA,in Pd/C catalyst and hydrochloric acid system.However,the catalyst suffers from deactivation due to the exoistentce of liquid aicd.This work focus on the conversion of FFA into 2-MF and the following transformation of 2-MF into 3-AP.The main conclusions are as follows:(1)Cu/SiO2 catalysts are prepared by co-precipitation method(CP)and ammonia evaporation method(AE)for vapor-phase hydrodeoxygenation of FFA to 2-MF.The results show that the products over Cu/SiO2(CP)catalyst are mainly 80%furfuryl alcohol along with 5%tetrahydrofurfuryl alcohol.However,the selectivity of 2-MF is higher than 86%with almost 100%conversion of FFA over Cu/SiO2(AE)catalyst.The structural characterization of the two catalysts show that the copper phyllosilicate structure is formed during the preparation process of Cu/SiO2(AE)catalyst,leading to the smaller metal nanoparctiles formed and easier reducibility.In addition,the special structure also promotes the synergistic effect between Cu0/Cu+,and the Cu+ site improves the surface acidity of the catalyst.The highly dispersed metal sites and the presence of Cu+ facilitate the formation of 2-MF.(2)The catalytic performance of Metal/Zeolite catalysts for the conversion of 2MF to 3-AP are studied.The experimental results show that the bifunctional catalyst Pd/HZSM-5 shows the best catalytic performance for the catalytic conversion of 3-AP from 2-MF at 98.2%conversion and 72.1%selectivity.On this basis,we prepare the encapsulated catalyst Pd@HZSM-5 by in situ synthesis,which achieve complete conversion of 2-MF with a selectivity of 90.6%of 3-AP.The characterization results confirm that due to the confinement of the molecular sieve channels,the metal dispersion of Pd@HZSM-5 catalyst is high,the particle size of Pd nanoparticles is small,and the amount of catalyst acid is significantly increased.The matching between metal/acid sites improves the catalytic performance of the bifunctional catalyst.In addition,the encapsulated catalyst Pd@HZSM-5 improves the cycling performance.